Carbonized Silk Nanofiber Membrane for Transparent and Sensitive Electronic Skin

Recent years have witnessed the explosive development of electronic skin. Highly sensitive pressure sensing is one of the primary abilities of electronic skin. To date, most of the reported skin‐like pressure sensors are based on nanomaterials and microstructured polydimethylsiloxane (PDMS) films, limiting their wide practical applications due to the unknown biotoxicity and the redundant fabrication procedure. A cost‐effective, large‐area‐capable, and biocompatible approach for fabrication of high‐performance skin‐like pressure sensors is highly desired. Silk fibroin (SF) is a natural protein that has recently drawn great attention due to its application as the substrate for flexible electronics. Here, the fabrication of skin‐like pressure sensors is demonstrated using SF‐derived active materials. Flexible and conformal pressure sensors can be fabricated using transparent carbonized silk nanofiber membranes (CSilkNM) and unstructured PDMS films through a cost‐effective and large‐scale capable approach. Due to the unique N‐doped carbon nanofiber network structure of CSilkNM, the obtained pressure sensor shows superior performance, including ultrahigh sensitivity (34.47 kPa^?1) for a broad pressure range, an ultralow detection limit (0.8 Pa), rapid response time (<16.7 ms), and high durability (>10 000 cycles). Based on its superior performance, its applications in monitoring human physiological signals, sensing subtle touch, and detecting spatial distribution of pressure are demonstrated.     

Highly Elastic Graphene‐Based Electronics Toward Electronic Skin

Epidermal electronics are extensively explored as an important platform for future biomedical engineering. Epidermal devices are typically fabricated using high‐cost methods employing complex vacuum microfabrication processes, limiting their widespread potential in wearable electronics. Here, a low‐cost, solution‐based approach using electroconductive reduced graphene oxide (RGO) sheets on elastic and porous poly(dimethylsiloxane) (PDMS) thin films for multifunctional, high‐performance, graphene‐based epidermal bioelectrodes and strain sensors is presented. These devices are fabricated employing simple coatings and direct patterning without using any complicated microfabrication processes. The graphene bioelectrodes show a superior stretchability (up to 150% strain), with mechanical durability up to 5000 cycles of stretching and releasing, and low sheet resistance (1.5 kΩ per square), and the graphene strain sensors exhibit a high sensitivity (a gauge factor of 7 to 173) with a wide sensing range (up to 40% strain). Fully functional applications of dry bioelectrodes in monitoring human electrophysiological signals (i.e., electrocardiogram, electroencephalography, and electromyogram) and highly sensitive strain sensors for precise detection of large‐scale human motions are demonstrated. It is believed that our unique processing capability and multifunctional device platform based on RGO/porous PDMS will pave the way for low‐cost processing and integration of 2D materials for future wearable electronic skin.     

Polyelectrolyte Dielectrics for Flexible Low‐Voltage Organic Thin‐Film Transistors in Highly Sensitive Pressure Sensing

Organic thin‐film transistors (OTFTs) can provide an effective platform to develop flexible pressure sensors in wearable electronics due to their good signal amplification function. However, it is particularly difficult to realize OTFT‐based pressure sensors with both low‐voltage operation and high sensitivity. Here, controllable polyelectrolyte composites based on poly(ethylene glycol) (PEG) and polyacrylic acid (PAA) are developed as a type of high‐capacitance dielectrics for flexible OTFTs and ultrasensitive pressure sensors with sub‐1 V operation. Flexible OTFTs using the PAA:PEG dielectrics show good universality and greatly enhanced electrical performance under a much smaller operating voltage of ?0.7 V than those with a pristine PAA dielectric. The low‐voltage OTFTs also exhibit excellent flexibility and bending stability under various bending radii and long cycles. Flexible OTFT‐based pressure sensors with low‐voltage operation and superhigh sensitivity are demonstrated by using a suspended semiconductor/dielectric/gate structure in combination with the PAA:PEG dielectric. The sensors deliver a record high sensitivity of 452.7 kPa^?1 under a low‐voltage of ?0.7 V, and excellent operating stability over 5000 cycles. The OTFT sensors can be built into a wearable sensor array for spatial pressure mapping, which shows a bright potential in flexible electronics such as wearable devices and smart skins.     

Flexible and Multifunctional Silk Textiles with Biomimetic Leaf‐Like MXene/Silver Nanowire Nanostructures for Electromagnetic Interference Shielding,Humidity Monitoring,and Self‐Derived Hydrophobicity

Although flexible and multifunctional textiles are promising for wearable electronics and portable device applications, the main issue is to endow textiles with multifunctionalities while maintaining their innate flexible and porous features. Herein, a vacuum‐assisted layer‐by‐layer assembly technique is demonstrated to conformally deposit electrically conductive substances on textiles for developing multifunctional and flexible textiles with superb electromagnetic interference (EMI) shielding performances, superhydrophobicity, and highly sensitive humidity response. The formed leaf‐like nanostructure is composed of silver nanowires (AgNWs) as the highly conductive skeleton (vein) and transition metal carbide/carbonitride (MXene) nanosheets as the lamina. The presence of MXene protects AgNWs from oxidation and enhances the combination of AgNWs with the fabric substrate, and the transformation of its functional groups leads to self‐derived hydrophobicity. The flexible and multifunctional textile exhibits a low sheet resistance of 0.8 Ω sq^?1, outstanding EMI shielding efficiency of 54 dB in the X‐band at a small thickness of 120 µm, and highly sensitive humidity responses, while retaining its satisfactory porosity and permeability. The self‐derived hydrophobicity with a large contact angle of >140° is achieved by aging the hydrophilic MXene coated silk. The wearable multifunctional textiles are highly promising for applications in intelligent garments, humidity sensors, actuators, and EMI shielding.     

Bioinspired Interlocked and Hierarchical Design of ZnO Nanowire Arrays for Static and Dynamic Pressure‐Sensitive Electronic Skins

The development of electronic skin (e‐skin) is of great importance in human‐like robotics, healthcare, wearable electronics, and medical applications. In this paper, a bioinspired e‐skin design of hierarchical micro‐ and nano‐structured ZnO nanowire (NW) arrays in an interlocked geometry is suggested for the sensitive detection of both static and dynamic tactile stimuli through piezoresistive and piezoelectric transduction modes, respectively. The interlocked hierarchical structures enable a stress‐sensitive variation in the contact area between the interlocked ZnO NWs and also the efficient bending of ZnO NWs, which allow the sensitive detection of both static and dynamic tactile stimuli. The flexible e‐skin in a piezoresistive mode shows a high pressure sensitivity (?6.8 kPa^?1) and an ultrafast response time (<5 ms), which enables the detection of minute static pressure (0.6 Pa), vibration level (0.1 m s^?2), and sound pressure (≈57 dB). The flexible e‐skin in a piezoelectric mode is also demonstrated to be able to detect fast dynamic stimuli such as high frequency vibrations (≈250 Hz). The flexible e‐skins with both piezoresistive and piezoelectric sensing capabilities may find applications requiring both static and dynamic tactile perceptions such as robotic hands for dexterous manipulations and various healthcare monitoring devices.     

Flexible Multifunctionalized Carbon Nanotubes‐Based Hybrid Nanowires

In this work, flexible multifunctionalized carbon nanotube (CNT)‐based hybrid nanowires are synthesized through surface modification processes. The good dispersability of the hybrid nanowire in polar solvents facilitates directly making fine patterns with a minimum width of 40 μm for applications of flexible and stretchable circuits (FSCs). The hybrid nanowire possesses a flexible and highly conductive structure which demonstrates stable electro‐mechanical properties on polydimethylsiloxane (PDMS) substrates under large structural deformation. FSCs fabricated from the hybrid nanowires show a constant resistance of 0.096 Ω □^?1 (equivalent of a resistivity 0.96 Ω μm) under repeated bending cycles. The FSCs also have a low and stable sheet resistance of 0.4 Ω □^?1 for strains up to 30%, which is almost four orders of magnitude lower than that of pure CNT samples (1316 Ω □^?1). Further improved stretchability and electro‐mechanical properties (0.1 Ω □^?1, at the strain of 100%) are achieved with a prestrain PDMS substrate. Repeated deformation tests demonstrate the high reliability of FSCs. The observed stable and reliable electro‐mechanical performance of FSCs suggests the potential use of the material in wearable and portable electronics.     

Large‐Area Ultrathin Graphene Films by Single‐Step Marangoni Self‐Assembly for Highly Sensitive Strain Sensing Application

Promoted by the demand for wearable devices, graphene has been proved to be a promising material for potential applications in flexible and highly sensitive strain sensors. However, low sensitivity and complex processing of graphene retard the development toward the practical applications. Here, an environment‐friendly and cost‐effective method to fabricate large‐area ultrathin graphene films is proposed for highly sensitive flexible strain sensor. The assembled graphene films are derived rapidly at the liquid/air interface by Marangoni effect and the area can be scaled up. These graphene‐based strain sensors exhibit extremely high sensitivity with gauge factor of 1037 at 2% strain, which represents the highest value for graphene platelets at this small deformation so far. This simple fabrication for strain sensors with highly sensitive performance of strain sensor makes it a novel approach to applications in electronic skin, wearable sensors, and health monitoring platforms.     

3D Graphene Films Enable Simultaneously High Sensitivity and Large Stretchability for Strain Sensors

Integration of 2D membranes into 3D macroscopic structures is essential to overcome the intrinsically low stretchability of graphene for the applications in flexible and wearable electronics. Herein, the synthesis of 3D graphene films (3D‐GFs) using chemical vapor deposition (CVD) is reported, in which a porous copper foil (PCF) is chosen as a template in the atmospheric‐pressure CVD preparation. When the 3D‐GF prepared at 1000 °C (noted as 3D‐GF‐1000) is transferred onto a polydimethylsiloxane (PDMS) membrane, the obtained 3D‐GF‐1000/PDMS hybrid film shows an electrical conductivity of 11.6 S cm^?1 with good flexibility, indicated by small relative resistance changes (ΔR/R₀) of 2.67 and 0.36 under a tensile strain of 50% and a bending radius of 1.6 mm, respectively. When the CVD temperature is reduced to 900 °C (generating a sample noted as 3D‐GF‐900), the 3D‐GF‐900/PDMS hybrid film exhibits an excellent strain‐sensing performance with a workable strain range of up to 187% and simultaneously a gauge factor of up to ≈1500. The 3D‐GF‐900/PDMS also shows a remarkable durability in resistance in repeated 5000 stretching‐releasing cycles. Kinetics studies show that the response of ΔR/R₀ upon strain is related to the graphitization and conductivity of 3D‐GF which are sensitive to the CVD preparation temperature.     

Seriography‐Guided Reduction of Graphene Oxide Biopapers for Wearable Sensory Electronics

Novel nacre‐mimic bio‐nanocomposites, such as graphene‐based laminates, are pushing the boundaries of strength and toughness as flexible engineering materials. Translating these material advances to functional flexible electronics requires methods for generating print‐scalable microcircuits (conductive elements surrounded by dielectric) into these strong, tough, lightweight bio‐nanocomposites. Here, a new paradigm for printing flexible electronics by employing facile, eco‐friendly seriography to confine the reduction of graphene oxide biopapers reinforced by silk interlayers is presented. Well‐defined, micropatterned regions on the biopaper are chemically reduced, generating a 10⁶ increase in conductivity (up to 10⁴ S m^?1). Flexible, robust graphene‐silk circuits are showcased in diverse applications such as resistive moisture sensors and capacitive proximity sensors. Unlike conductive (i.e., graphene‐ or Ag nanoparticle‐loaded) inks printed onto substrates, seriography‐guided reduction does not create mechanically weak interfaces between dissimilar materials and does not require the judicious formation of ink. The unimpaired functionality of printed‐in graphene‐silk microcircuits after thousands of punitive folding cycles and chemical attack by harsh solvents is demonstrated. This novel approach provides a low‐cost, portable solution for printing micrometer‐scale conductive features uniformly across large areas (>hundreds of cm²) in layered composites for applications including wearable health monitors, electronic skin, rollable antennas, and conformable displays.     

Conductive Hierarchical Hairy Fibers for Highly Sensitive,Stretchable, and Water‐Resistant Multimodal Gesture‐Distinguishable Sensor,VR Applications

Conductive fibers, which are highly adaptable to the morphologies of the human body, are attractive for the development of wearable systems, smart clothing, and textronics to detect various biological signals and human motions. A fiber‐based conductive sensor interconnected with hierarchical microhairy architectures, exhibiting remarkable stretchability (<200%) and sensitivity for various stimuli (pressure, stretching, and bending), is developed. For distinguishability of multiple gestures, two hierarchical hairy conductive fibers are twisted to fabricate a fiber‐type sensor, which monitors distinct waveforms of electrical signals retrieved from pressure, stretching, and bending. This sensor is highly robust under repeated appliances of external stimuli over multiple cyclic tests of various modes (<2200 cycles for each stimulus). Upon formation of a self‐assembled monolayer, it exhibits stable performance even under wet conditions. For practical applications, this sensor can be weaved into a smart glove to demonstrate a pressure and gesture‐discernible wearable controller for virtual reality (VR) interface, shedding light on advances in wearable electronics with medical and healthcare functionalities and VR systems.     

All‐Printed Flexible and Stretchable Electronics with Pressing or Freezing Activatable Liquid‐Metal–Silicone Inks

Liquid‐metal (LM)‐based flexible and stretchable electronics have attracted widespread interest in wearable computing, human–machine interaction, and soft robotics. However, many current examples are one‐off prototypes, whereas future implementation requires mass production. To address this critical challenge, an integrated multimaterial 3D printing process composed of direct ink writing (DIW) of sealing silicone elastomer and special LM‐silicone (LMS) inks for manufacturing high‐performance LM‐based flexible and stretchable electronics is presented. The LMS ink is a concentrated mixture of LM microdroplets and silicone elastomer and exhibits excellent printability for DIW printing. Guided by a verified theoretical model, a printing process with high resolution and high speed can be easily implemented. Although LMS is not initially conductive, it can be activated by pressing or freezing. Activated LMS possesses good conductivity and significant electrical response to strain. Owing to LMS's unique structure, LMS‐embedded flexible electronics exhibit great damage mitigation, in that no leaking occurs even when damaged. To demonstrate the flexibility of this process in fabricating LM‐based flexible electronics, multilayer soft circuits, strain sensors, and data gloves are printed and investigated. Notably, utilizing LMS's unique activating property, some functional circuits such as one‐time pressing/freezing‐on switch can be printed without any structural design.     

Spray‐Layer‐by‐Layer Carbon Nanotube/Electrospun Fiber Electrodes for Flexible Chemiresistive Sensor Applications

Development of a versatile method for incorporating conductive materials into textiles could enable advances in wearable electronics and smart textiles. One area of critical importance is the detection of chemicals in the environment for security and industrial process monitoring. Here, the fabrication of a flexible, sensor material based on functionalized multi‐walled carbon nanotube (MWNT) films on a porous electrospun fiber mat for real‐time detection of a nerve agent simulant is reported. The material is constructed by layer‐by‐layer (LbL) assembly of MWNTs with opposite charges, creating multilayer films of MWNTs without binder. The vacuum‐assisted spray‐LbL process enables conformal coatings of nanostructured MWNT films on individual electrospun fibers throughout the bulk of the mat with controlled loading and electrical conductivity. A thiourea‐based receptor is covalently attached to the primary amine groups on the MWNT films to enhance the sensing response to dimethyl methylphosphonate (DMMP), a simulant for sarin nerve agent. Chemiresistive sensors based on the engineered textiles display reversible responses and detection limits for DMMP as low as 10 ppb in the aqueous phase and 5 ppm in the vapor phase. This fabrication technique provides a versatile and easily scalable strategy for incorporating conformal MWNT films into three‐dimensional substrates for numerous applications.     

Self‐Powered Electronics by Integration of Flexible Solid‐State Graphene‐Based Supercapacitors with High Performance Perovskite Hybrid Solar Cells

To develop high‐capacitance flexible solid‐state supercapacitors and explore its application in self‐powered electronics is one of ongoing research topics. In this study, self‐stacked solvated graphene (SSG) films are reported that have been prepared by a facile vacuum filtration method as the free‐standing electrode for flexible solid‐state supercapacitors. The highly hydrated SSG films have low mass loading, high flexibility, and high electrical conductivity. The flexible solid‐state supercapacitors based on SSG films exhibit excellent capacitive characteristics with a high gravimetric specific capacitance of 245 F g^?1 and good cycling stability of 10 000 cycles. Furthermore, the flexible solid‐state supercapacitors are integrated with high performance perovskite hybrid solar cells (pero‐HSCs) to build self‐powered electronics. It is found that the solid‐state supercapacitors can be charged by pero‐HSCs and discharged from 0.75 V. These results demonstrate that the self‐powered electronics by integration of the flexible solid‐state supercapacitors with pero‐HSCs have great potential applications in storage of solar energy and in flexible electronics, such as portable and wearable personal devices.     

MXene Functionalized,Highly Breathable and Sensitive Pressure Sensors with Multi-Layered Porous Structure

Breathable, flexible, and highly sensitive pressure sensors have drawn increasing attention due to their potential in wearable electronics for body-motion monitoring, human-machine interfaces, etc. However, current pressure sensors are usually assembled with polymer substrates or encapsulation layers, thus causing discomfort during wearing (i.e., low air/vapor permeability, mechanical mismatch) and restricting their applications. A breathable and flexible pressure sensor is reported with nonwoven fabrics as both the electrode (printed with MXene interdigitated electrode) and sensing (coated with MXene/silver nanowires) layers via a scalable screen-printing approach. Benefiting from the multi-layered porous structure, the sensor demonstrates good air permeability with high sensitivity (770.86–1434.89 kPa⁻¹), a wide sensing range (0–100 kPa), fast response/recovery time (70/81 ms), and low detection limit (≈1 Pa). Particularly, this sensor can detect full-scale human motion (i.e., small-scale pulse beating and large-scale walking/running) with high sensitivity, excellent cycling stability, and puncture resistance. Additionally, the sensing layer of the pressure sensor also displays superior sensitivity to humidity changes, which is verified by successfully monitoring human breathing and spoken words while wearing a sensor-embedded mask. Given the outstanding features, this breathable sensor shows promise in the wearable electronic field for body health monitoring, sports activity detection, and disease diagnosis.     

Super-Stretchable,Anti-Freezing,Anti-Drying Organogel Ionic Conductor for Multi-Mode Flexible Electronics

Due to their intrinsic flexibility, tunable conductivity, multiple stimulus-response, and self-healing ability, ionic conductive hydrogels have drawn significant attention in flexible/wearable electronics. However, challenges remain because traditional hydrogels inevitably faced the problems of losing flexibility and conductivity because of the inner water loss when exposed to the ambient environment. Besides, the water inside the hydrogel will freeze at the water icing temperatures, making the device hard and fragile. As a promising alternative, organogels have attracted wide attention because they can, to some extent, overcome the above drawbacks. Herein, a kind of organogel ionic conductor (MOIC) by a self-polymerization reaction is involved, which is super stretchable, anti-drying, and anti-freezing. Meanwhile, it can still maintain high mechanical stability after alternately loading/unloading at the strain of 600% for 600 s (1800 cycles). Using this MOIC, high-performance triboelectric nanogenerator (TENG) is constructed (MOIC-TENG) to harvest small mechanical energy even the MOIC electrode underwent an extremely low temperature. In addition, multifunctional flexible/wearable sensors (strain sensor, piezoresistive sensor, and tactile sensor) are realized to monitor human motions in real time, and recognize different materials by triboelectric effect. This study demonstrates a promising candidate material for flexible/wearable electronics such as electronic skin, flexible sensors, and human-machine interfaces.     

Conductive PEDOT:PSS on surface-functionalized chitosan biopolymers for stretchable skin-like electronics

Poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) is a promising alternative transparent electrode to replace conventional indium tix oxide (ITO) for flexible and stretchable electronics. For their applications in optoelectronic devices, realizing both high conductivity and transmittance for the films is of great necessity as a suitable high performance transparent electrode. Here, we demonstrate simultaneously enhanced electrical and optical properties of PEDOT:PSS films prepared on chitosan bio-substrates by using an organic surface modifier, 11-aminoundecanoic acid (11-AA). The sheet resistance of PEDOT:PSS films decreases from 1120.8 to 292.8 Ω/sq with an increase in a transmittance from 75.9 to 80.4% by 11-AA treatment on the chitosan films. The functional groups of 11-AA effectively enhance the adhesion property at the interface between the chitosan substrate and PEDOT:PSS by forming strong interfacial bondings and decrease insulating PSS from PEDOT:PSS films. The wearable heater devices and on-skin sensors based on the 11-AA-treated PEDOT:PSS on the chitosan bio-substrates are successfully fabricated, showing the excellent thermal and sensing performances. The 11-AA surface-modification approach for highly conductive PEDOT:PSS on chitosan bio-substrates presents a great potential for applications toward transparent, flexible and stretchable electronics.     

Light‐Boosting Highly Sensitive Pressure Sensors Based on Bioinspired Multiscale Surface Structures

Pressure sensors have attracted tremendous attention because of their potential applications in the fields of health monitoring, human–machine interfaces, artificial intelligence, and so on. Improving pressure‐sensing performances, especially the sensitivity and the detection limit, is of great importance to expand the related applications, however it is still an enormous challenge so far. Herein, highly sensitive piezoresistive pressure sensors are reported with novel light‐boosting sensing performances. Rose petal–templated positive multiscale millimeter/micro/nanostructures combined with surface wrinkling nanopatterns endow the assembled pressure sensors with outstanding pressure sensing performance, e.g. an ultrahigh sensitivity (70 KPa^?1, <0.5 KPa), an ultralow detection limit (0.88 Pa), a wide pressure detect ion range (from 0.88 Pa to 32 KPa), and a fast response time (30 ms). Remarkably, simple light illumination further enhances the sensitivity to 120 KPa^?1 (<0.5 KPa) and lowers the detection limit to 0.41 Pa. Furthermore, the flexible light illumination offers unprecedented capabilities to spatiotemporally control any target in multiplexed pressure sensors for optically enhanced/tailorable sensing performances. This light‐control strategy coupled with the introduction of bioinspired multiscale structures is expected to help design next generation advanced wearable electronic devices for unprecedented smart applications.     

Microporous Polypyrrole‐Coated Graphene Foam for High‐Performance Multifunctional Sensors and Flexible Supercapacitors

This study reports on the fabrication of pressure/temperature/strain sensors and all‐solid‐state flexible supercapacitors using only polydimethylsiloxane coated microporous polypyrrole/graphene foam composite (PDMS/PPy/GF) as a common material. A dual‐mode sensor is designed with PDMS/PPy/GF, which measures pressure and temperature with the changes of current and voltage, respectively, without interference to each other. The fabricated dual‐mode sensor shows high sensitivity, fast response/recovery, and high durability during 10 000 cycles of pressure loading. The pressure is estimated using the thermoelectric voltage induced by simultaneous increase in temperature caused by a finger touch on the sensor. Additionally, a resistor‐type strain sensor fabricated using the same PDMS/PPy/GF could detect the strain up to 50%. Flexible, high performance supercapacitor used as a power supply is fabricated with electrodes of PPy/GF for its high surface area and pseudocapacitance. Furthermore, an integrated system of such fabricated multifunctional sensors and a supercapacitor on a skin‐attachable flexible substrate using liquid–metal interconnections operates well, whereas sensors are driven by the power of the supercapacitor. This study clearly demonstrates that the appropriate choice of a single functional material enables fabrication of active multifunctional sensors for pressure, temperature, and strain, as well as the supercapacitor, that could be used in wirelessly powered wearable devices.     

Stretchable,Skin‐Mountable,and Wearable Strain Sensors and Their Potential Applications: A Review

There is a growing demand for flexible and soft electronic devices. In particular, stretchable, skin‐mountable, and wearable strain sensors are needed for several potential applications including personalized health‐monitoring, human motion detection, human‐machine interfaces, soft robotics, and so forth. This Feature Article presents recent advancements in the development of flexible and stretchable strain sensors. The article shows that highly stretchable strain sensors are successfully being developed by new mechanisms such as disconnection between overlapped nanomaterials, crack propagation in thin films, and tunneling effect, different from traditional strain sensing mechanisms. Strain sensing performances of recently reported strain sensors are comprehensively studied and discussed, showing that appropriate choice of composite structures as well as suitable interaction between functional nanomaterials and polymers are essential for the high performance strain sensing. Next, simulation results of piezoresistivity of stretchable strain sensors by computational models are reported. Finally, potential applications of flexible strain sensors are described. This survey reveals that flexible, skin‐mountable, and wearable strain sensors have potential in diverse applications while several grand challenges have to be still overcome.     

Template‐Directed Growth of Hierarchical MOF Hybrid Arrays for Tactile Sensor

Recently, conductive metal?organic frameworks (MOFs) as the active material have provided broad prospects for electronic device application. The positioning technologies for MOFs enable the fabrication of novel microstructures, which can modulate the morphology of the material and tune the properties for the targeted application. Herein, a template‐method is used to synthesize the hierarchical structure of MOF hybrid array (MHA) on copper mesh (MHA@Mesh) for flexible sensor. Finite element method (FEM) results indicate that the 3D hierarchical MHA@Mesh can mimic the micro/nanoscale structure of human skin, which enables an interlocking contact. MHA@Mesh‐based flexible sensor presents rapid response rate (<1 ms) and high sensitivity (up to 307 kPa^?1) which is 20 times higher than that of MHA@Foil‐based sensor (15 kPa^?1). The flexible pressure device could be applied to monitor the finger motion and human pulses. Moreover, the music recognition can be performed by integrating the MOFs hardware sensors with machine learning algorithms. Overall, this design concept of 3D hierarchical microarray structures demonstrates potential in the fields of wearable technologies and human–machine interfaces.