Construction of Flexible Piezoceramic Array with Ultrahigh Piezoelectricity via a Hierarchical Design Strategy

The µW-level power density of flexible piezoelectric energy harvesters (FPEHs) restricts their potential in applications related to high-power multifunctional wearable devices. To overcome this challenge, a hierarchical design strategy is proposed by forming porous piezoceramics with an optimum microstructure into an ordered macroscopic array structure to enable the construction of high performance FPEHs. The porous piezoceramic elements allows optimization of the sensing and harvesting Figure of merit, and the array structure causes a high level of effective strain under a mechanical load. The introduction of a network of polymer channels between the piezoceramic array also provides increased device flexibility, thereby allowing the device to attach and conform to the curved contours of the human body. The unique hierarchical piezoceramic array architecture exhibits superior flexibility, a high open circuit voltage (618 V), high short circuit current (188 µA), and ultrahigh power density (19.1 mW cm⁻²). This energy density value surpasses previously reported high-performance FPEHs. The ultrahigh power flexible harvesting can charge a 0.1 F supercapacitor at 2.5 Hz to power high-power electronic devices. Finally, the FPEH is employed in two novel applications related to fracture healing monitoring and self-powered wireless position tracking in extreme environments.     

Transparent,Flexible, and Highly Sensitive Piezocomposite Capable of Harvesting and Monitoring Kinetic Movements of Microbubbles in Liquid

In this study, a zinc oxide (ZnO)-decorated nickel microfiber (ZNMF)-based piezoelectric nanogenerator (ZNMF-PENG) using electrospinning, metal electroplating, electrospraying, and ceramic growing techniques is fabricated. The combination of these techniques enables the ZNMF-PENG to possess high transparency and flexibility that are difficult to achieve through the existing piezoceramic-based PENGs. In particular, the presence of innumerable piezoceramic ZnO nanowires inside the ZNMF-PENG allows for detecting microbubble movements having an extremely low buoyancy force of 0.009 N, which is beneficial for detecting cavitation. Moreover, in comparison to previously reported PENGs fabricated using an electrospinning technique, the ZNMF-PENG demonstrates the highest energy-harvesting efficiency of 8750 V N⁻¹ m⁻². The novel approach in materials and methods proposed in this study is expected to contribute to the further advancement in developing transparent, flexible, and performance-improved PENGs applicable to various industrial applications.     

Ultrahigh-Areal Capacitance Flexible Supercapacitors Based on Laser Assisted Construction of Hierarchical Aligned Carbon Nanotubes

Electrochemical energy storage is a key technology for a clean and sustainable energy supply. In this respect, supercapacitors (SC) have recently received considerable attention due to their excellent performance, including high-power density and long-cycle life. However, the poor binding strength between the active materials and substrate, the low active material loading, and small specific capacitance hinder the overall performance improvement of the device. In this study, an ultrahigh-areal capacitance flexible SC based on the Al micro grid-based hierarchical vertically aligned carbon nanotubes (VACNTs) is studied. Interestingly, the Al micro grid-based VACNTs exhibit ultrahigh loading (13 mg cm⁻²), and the as-fabricated VACNTs electrode display outstanding electrochemical performance, including an impressive areal capacitance of 1,300 mF cm⁻² at the current density of 13 mA cm⁻² and excellent stability with a retention ratio of 90% after 20,000 cycles at the current density of 130 mA cm⁻². Furthermore, the hierarchical VACNT electrodes show excellent mechanical flexibility when assembled into quasi-solid-state SC using Na₂SO₄-PVA gel as the electrolyte. The capacitance of this device is hardly changed bending different angles, even 180°. This study demonstrates the tremendous potential of Al micro grid-based hierarchical VACNTs as electrodes for high-performance flexible and wearable energy storage devices.     

Bioinspired and Hierarchically Textile-Structured Soft Actuators for Healthcare Wearables

Soft pneumatic actuators possess the increasing potential for various healthcare applications, such as smart wearable devices, safe human-robot interaction, and flexible manipulators. However, it is difficult to translate the existing technologies to commercial applications due to their inefficient volumetric power, sophisticated control with high operation pressure, slow production, and high cost. To overcome these issues, herein, a caterpillar-inspired actuator using hierarchical textile architectures based on simple fabrication and low-cost strategy is designed. Unlike the existing textile-based pneumatic actuators, the designed actuators are constructed by combining boucle fancy yarns with a novel trilayer-knit architecture. The as-prepared actuators concurrently possess fast response (1100° s⁻¹), large bending actuation strain (1080° m⁻¹), high-power density (272 W m⁻³), mechanical robustness, easy-programmable motions, and human-tactile comfort, which outperforms currently reported textile-based pneumatic actuators. Furthermore, due to the geometrical transition of the engineered hierarchical structure, the developed actuators exhibit superior dual-stiffness effect with stress evolution, providing a facile approach to addressing the conflict of flexibility and force output in soft fluidic actuators. This concept as a paradigm provides new insights to develop soft actuators with outstanding design flexibility, adaptability, and multifunctionality using engineered textile-structure, which has great potential for real-world applications in medical rehabilitation, physiotherapy, and soft robotics.     

A Biomimetic Transpiration Textile for Highly Efficient Personal Drying and Cooling

Efficient sweat release and heat dissipation are required for functional textiles that improve comfort and productivity while being worn in daily life. However, the porous structure of textiles exhibits an opposite effect on water transport and heat transfer capacities, leading to a longstanding bottleneck for the design of multifunctional drying and cooling textiles. Here, a biomimetic transpiration textile based on the hierarchical and interconnected network of vascular plants is demonstrated for highly efficient personal drying and cooling. The transpiration-inspired design offers a textile with distinct advantages, including a desired one-way water transport index (1072%), rapid water evaporation rate (0.36 g h⁻¹), and outstanding through-plane (0.182 W m⁻¹ K⁻¹) and in-plane (1.137 W m⁻¹ K⁻¹) thermal conductivities. Moreover, based on the optimized performance, plausible mechanisms are proposed and calculated to provide insight into the water transport and heat transfer within the hierarchical and interconnected network, which provide promising benefits to the development of multifunctional drying and cooling textiles. Overall, the successful synthesis of this biomimetic transpiration textile provides a comfortable microclimate to the human body, thus satisfying the growing demand for better health, productivity, and sustainability.     

Muscle Fibers Inspired High-Performance Piezoelectric Textiles for Wearable Physiological Monitoring

The next-generation wearable biosensors with highly biocompatible, stretchable, and robust features are expected to enable the change of the current reactive and disease-centric healthcare system to a personalized model with a focus on disease prevention and health promotion. Herein, a muscle-fiber-inspired nonwoven piezoelectric textile with tunable mechanical properties for wearable physiological monitoring is developed. To mimic the muscle fibers, polydopamine (PDA) is dispersed into the electrospun barium titanate/polyvinylidene fluoride (BTO/PVDF) nanofibers to enhance the interfacial-adhesion, mechanical strength, and piezoelectric properties. Such improvements are both experimentally observed via mechanical characterization and theoretically verified by the phase-field simulation. Taking the PDA@BTO/PVDF nanofibers as the building blocks, a nonwoven light-weight piezoelectric textile is fabricated, which hold an outstanding sensitivity (3.95 V N⁻¹) and long-term stability (<3% decline after 7,400 cycles). The piezoelectric textile demonstrates multiple potential applications, including pulse wave measurement, human motion monitoring, and active voice recognition. By creatively mimicking the muscle fibers, this work paves a cost-effective way to develop high-performance and self-powered wearable bioelectronics for personalized healthcare.     

A Flexible and Safe Planar Zinc-Ion Micro-Battery with Ultrahigh Energy Density Enabled by Interfacial Engineering for Wearable Sensing Systems

Aqueous zinc-ion micro-batteries (ZIMBs) have attracted considerable attention owing to their reliable safety, low cost, and great potential for wearable devices. However, current ZIMBs still suffer from various critical issues, including short cycle life, poor mechanical stability, and inadequate energy density. Herein, the fabrication of flexible planar ZIMBs with ultrahigh energy density by interfacial engineering in the screen-printing process based on high-performance MnO₂-based cathode materials is reported. The Ce-doped MnO₂ (Ce-MnO₂) exhibits significantly enhanced capacity (389.3 mAh g⁻¹), considerable rate capability and admirable cycling stability than that of the pure MnO₂. Importantly, the fabrication of micro-electrodes with ultrahigh mass loading of Ce-MnO₂ (24.12 mg cm⁻²) and good mechanical stability is achieved through optimizing the interfacial bonding between different printed layers. The fabricated planar ZIMBs achieve a record high capacity (7.21 mAh cm⁻² or 497.31 mAh cm⁻³) and energy density (8.43 mWh cm⁻² or 573.45 mWh cm⁻³), as well as excellent flexibility. Besides, a wearable self-powered sensing system for environmental monitoring is further demonstrated by integrating the planar ZIMBs with flexible solar cells and a multifunctional sensor array. This work sheds light on the development of high-performance planar ZIMBs for future self-powered and eco-friendly smart wearable electronics.     

Nano-Engineered Carbon Fibre-Based Piezoelectric Smart Composites for Energy Harvesting and Self-Powered Sensing

The integration of piezoelectric materials onto carbon fiber (CF) can add energy harvesting and self-power sensing capabilities enabling great potential for “Internet of Things” (IoT) applications in motion tracking, environmental sensing, and personal portable electronics. Herein, a CF-based smart composite is developed by integrating piezoelectric poly(3,4-ethylenedioxythiophene) (PEDOT)/CuSCN-coated ZnO nanorods onto the CF surfaces with no detrimental effect on the mechanical properties of the composite, forming composites using two different polymer matrices: highly flexible polydimethylsiloxane (PDMS) and more rigid epoxy. The PDMS-coated piezoelectric smart composite can serve as an energy harvester and a self-powered sensor for detecting variations in impact acceleration with increasing output voltage from 1.4 to 7.6 V under impact acceleration from 0.1 to 0.4 m s⁻². Using epoxy as the matrix for a CF-reinforced plastic (CFRP) device with sensing and detection functions produces a voltage varying from 0.27 to 3.53 V when impacted at acceleration from 0.1 to 0.4 m s⁻², with a lower output compared to the PDMS-coated device attributed to the greater stiffness of the matrix. Finally, spatially sensitive detection is demonstrated by positioning two piezoelectric structures at different locations, which can identify the location as well as the level of the impacting force from the fabricated device.     

Multilevel Structure Engineered Lead-Free Piezoceramics Enabling Breakthrough in Energy Harvesting Performance for Bioelectronics

The prevalence of wearable/implantable medical electronics together with the rapid development of the Internet of Medicine Things call for the advancement of biocompatible, reliable, and high-efficiency energy harvesters. However, most current harvesters are based on toxic lead-based piezoelectric materials, raising biological safety concerns. What hinders the application of lead-free piezoelectric energy harvesters (PEHs) is the low power output, where the key challenge lies in obtaining a high piezoelectric voltage constant (g₃₃) and harvesting figure of merit (d₃₃ × g₃₃). Here, micron pores are introduced into phased boundary engineered high-performance (K, Na)NbO₃-based ceramic matrix, resulting in the state-of-the-art g₃₃ and the highest d₃₃ × g₃₃ values of 57.3 × 10⁻³ Vm N⁻¹ and 20887 × 10⁻¹⁵ m² N⁻¹ in lead-free piezoceramics, respectively. Concomitantly, ultrahigh energy harvesting performances are obtained in porous ceramic PEHs, with output voltage and power density of 200 V and 11.6 mW cm⁻² under instantaneous force impact and an average charging rate of 14.1 µW under high-frequency (1 MHz) ultrasound excitation, far outperforming previously reported PEHs. Porous ceramic PEHs are further developed into wearable and bio-implantable devices for human motion sensing and percutaneous ultrasound power transmission, opening avenues for the design of next-generation eco-friendly WIMEs.     

Rugged Soft Robots using Tough,Stretchable, and Self-Healable Adhesive Elastomers

Soft robots are susceptible to premature failure from physical damages incurred within dynamic environments. To address this, we report an elastomer with high toughness, room temperature self-healing, and strong adhesiveness, allowing both prevention of damages and recovery for soft robotics. By functionalizing polyurethane with hierarchical hydrogen bonds from ureido-4[1H]-pyrimidinone (UPy) and carboxyl groups, high toughness (74.85 MJ m⁻³), tensile strength (9.44 MPa), and strain (2340%) can be achieved. Furthermore, solvent-assisted self-healing at room temperature enables retention of high toughness (41.74 MJ m⁻³), tensile strength (5.57 MPa), and strain (1865%) within only 12 h. The elastomer possesses a high dielectric constant (≈9) that favors its utilization as a self-healing dielectric elastomer actuator (DEA) for soft robotics. Displaying high area strains of ≈31.4% and ≈19.3% after mechanical and electrical self-healing, respectively, the best performing self-healable DEA is achieved. With abundant hydrogen bonds, high adhesive strength without additional curing or heating is also realized. Having both actuation and adhesive properties, a “stick-on” strategy for the assembly of robust soft robots is realized, allowing soft robotic components to be easily reassembled or replaced upon severe damage. This study highlights the potential of soft robots with extreme ruggedness for different operating conditions.     

A Universal Aqueous Conductive Binder for Flexible Electrodes

The development of wearable electronics has led to new requirements for flexible and high-energy batteries. However, the conventional polyvinylidene fluoride binder fails in the manufacture of high-loaded and thick battery electrodes owing to its insufficient adhesiveness and electronic insulation, let alone for flexible devices. Furthermore, organic processing is expensive and not eco-friendly. Herein, the authors report a novel aqueous conductive binder made of carbon nanotubes interwoven in cellulose nanosheets, successfully satisfying the fabrication of flexible yet high-strength electrodes for universal active materials of different sizes, morphologies, and negative-to-positive working potentials, with a high mass loading of up to ≈ 90 mg cm⁻². The conductive binder has an ultrathin 2D-reticular nanosheet structure that forms continuous conductive skeletons in electrodes to segregate and warp active particles via a robust “face-to-point” bonding mode, allowing the fabricated electrodes to have remarkable flexibility and excellent mechanical integrity even under various external forces and excessive electrolyte erosion. Flexible LCO cathodes with a mass loading of > 30 mg cm⁻² as a case study exhibit high mechanical strength ( > 20 MPa) and can easily achieve an ultrahigh areal capacity of 12.1 mAh cm⁻². This cellulose-based binder system is ideal for advanced high-performance functional devices, especially for flexible and high-energy batteries.     

Interface Engineering of Biomass-Derived Carbon used as Ultrahigh-Energy-Density and Practical Mass-Loading Supercapacitor Electrodes

The development of flexible electrodes with high mass loading and efficient electron/ion transport is of great significance but still remains the challenge of innovating suitable electrode structures for high energy density application. Herein, for the first time, lignosulfonate-derived N/S-co-doped graphene-like carbon is in situ formed within an interface engineered cellulose textile through a sacrificial template method. Both experimental and theoretical calculations disclose that the formed pomegranate-like structure with continuous conductive pathways and porous characteristics allows sufficient ion/electron transport throughout the entire structures. As a result, the obtained flexible electrode delivers a remarkable integrated capacitance of 6534 mF cm⁻² (335.1 F g⁻¹) and a superior stability at an industrially applicable mass loading of 19.5 mg cm⁻². A pseudocapacitive cathode with ultrahigh capacitance of 7000 mF cm⁻² can also be obtained based on the same electrode structure engineering. The as-assembled asymmetric supercapacitor achieves a high areal capacitance of 3625 mF cm⁻², and a maximum energy density of 1.06 mWh cm⁻², outperforms most of other reported high-loading supercapacitors. This synthesis method and structural engineering strategy can provide materials design concepts and a wide range of applications in the fields of energy storage beyond supercapacitors.     

Highly Stretchable,Resilient, Adhesive,and Self-Healing Ionic Hydrogels for Thermoelectric Application

Harvesting low-grade waste heat from the natural environment with thermoelectric materials is considered as a promising solution for the sustainable energy supply for wearable electronic devices. For practical applications, it is desirable to endow the thermoelectric materials with excellent mechanical and self-healing properties, which remains a great challenge. Herein, the design and characterization of a series of high-performance ionic hydrogels for soft thermoelectric generator applications are reported. Composed of a physically cross-linked network of polyacrylic acid (PAA) and polyethylene glycol (PEO) doped with sodium chloride, the resulting PAA-PEO-NaCl ionic hydrogels demonstrates impressive mechanical strength (breaking stress >1.3 MPa), stretchability (>1100%), and toughness (up to 7.34 MJ m⁻³). Moreover, the reversible hydrogen bonding interaction and chain entanglement render the ionic hydrogels with excellent mechanical resilience, adhesion properties, and self-healing properties. At ambient conditions, the electrochemical and thermoelectric performance of the ionic hydrogels can be restored immediately from physical damage such as cutting, and the mechanical healing can be completely restored within 24 h. At the optimized composition, the Seebeck coefficient of the ionic hydrogels can reach 3.26 mV K⁻¹ with a low thermal conductivity of 0.321 W m⁻¹ K⁻¹. Considering the excellent mechanical properties and thermoelectric performance, it is believed that the ionic hydrogels are widely applicable in ionic thermoelectric capacitors to convert low-grade heat into electricity for soft electronic devices.     

Preparation and properties of electrically conductive,flexible and transparent silver nanowire/poly (lactic acid) nanocomposites

As the everyday use of petroleum-based products has raised environmental concerns, there is an urgent need to replace them with green materials. In this work, an eco-friendly, highly conductive, flexible silver nanowire/poly (lactic acid) film has been fabricated through a simple casting method by embedding the silver nanowires (AgNWs) below the surface of the poly lactic acid (PLA) matrix. The fabricated film has a high optical transparency of 89.5% with a sheet resistance of 64.8 Ω/□ and a figure of merit (FoM) of 4.92 × 10⁻³ Ω⁻¹ which is comparable to that of indium tin oxide (ITO). These films demonstrate excellent flexibility, great adhesion, smooth surface with root mean square (RMS) roughness of 11.7 nm and high mechanical properties with tensile strength and Young's modulus of 39.8 (MPa) and 1.6 (GPa). The results obtained from different testing methods show that the AgNW/PLA nanocomposites are potential candidates in flexible electronics and optoelectronics.     

Functionalized Poly(phenylene ether) with high thermal stability as flexible dielectrics and substrates for organic field-effect transistors

Extensive research efforts are devoted into seeking the thermally and mechanically durable dielectric materials for flexible electronics. In this work, a series of sulfonylated poly (phenylene ether)s (PPEs) were synthesized and served as gate dielectrics in the flexible OFET devices with crosslinked poly (2-allyl-6-methylphenol-co-2,6-dimethylphenol) (APPE) as substrate. The chemical structure, thermal, morphology, and dielectric properties were investigated, and the corresponding OFET devices were accordingly fabricated and characterized. We found that the discrepancy in sulfone content of PPE-xS renders the difference in thermal stability, surface polarity and dielectric constants. Among them, PPE-9kS with the highest sulfone content of 63% shows the best dielectric properties in the flexible OFET devices with hole mobility (μ_p) of 0.45 cm² V⁻¹ s⁻¹, outperforming its parent polymer without sulfone group (PPE-9k) with μ_p of 0.14 cm² V⁻¹ s⁻¹. Besides, the flexible device with PPE-9kS as dielectric exhibits highly retained device performance after cyclic bending or thermal treatment, which indicates the decent mechanical and thermal durability. The present study documents a practical methodology to fabricate a high-performance flexible OFET with excellent thermal and mechanical stability.     

Crocodile Skin-Inspired Protective Composite Textiles with Pattern-Controllable Soft-Rigid Unified Structures

Functional textiles with desirable protective properties (i.e., high cut-, stab-, and abrasion resistance) and wearability (i.e., excellent flexibility and permeability) remain unmet goals for personal protective equipment. Herein, inspired by crocodile skin, a unique and soft-rigid unified structure (SRUS) is reported by integrating rigid protective blocks onto a soft textile substrate while obtaining a high cut-, stab-, and abrasion-resistant composite textile that is flexible, waterproof, and breathable. Rigid blocks, consisting of epoxy resin reinforced by inorganic powders, strongly adhere to the soft textile surface with small intervals between each other via a pattern-controllable integrated molding (PCIM) approach. Consequently, the SRUS design guarantees superior protective performance through rigid protective blocks and satisfactory flexibility and permeability via soft textiles and intervals. The SRUS textile achieves excellent cut-resistance (58 N), the highest grades of stab- (38 N) and abrasion-resistance (600 r mg⁻¹), and good flexibility (65 mN cm) and permeability (60 mm s⁻¹) values, indicating a distinct combination of desirable protective and wearable performance. The proposed SRUS protective textiles, incorporating the PCIM approach, offer a novel strategy for manufacturing functional soft composite textiles that combine high protective performance and good wearability, opening up a new avenue for the development of personal protective equipment.     

Meso-Reconstruction of Silk Fibroin based on Molecular and Nano-Templates for Electronic Skin in Medical Applications

A unique strategy of mesoscopic functionalization starting from silk fibroin (SF) materials to the fabrication of meso flexible SF electronic skin (e-skin) is presented. Notably, SF materials of novel and enhanced properties of the materials can be achieved by mesoscopically reconstructing the hierarchical structures of SF materials, based on rerouting the refolding process of SF molecules by meso-nucleation templating. Mesoscopic hybridization/reconstruction endows cocoon silk with a robust mechanical and electric performance by incorporating wool keratin (WK) and carbon nanotubes (CNTs) into the mesostructures of SF via intermolecular templated nucleation. Furthermore, the asymmetrical meso-functional films with biocompatibility and insulation on one side and conductivity on the other (square resistance = 130 Ω sq⁻¹) endow the passive wireless e-skin exhibited a tunable sensitivity from −1.05 to −6.35 kPa⁻¹ with a lossless measurement range of ≈2 kPa. The pulses of human subjects are monitored using the e-skin to evaluate blood vessel hardening and real-time dynamic systolic and diastolic blood pressure.     

Industry-Scale and Environmentally Stable Ti3C2Tx MXene Based Film for Flexible Energy Storage Devices

MXenes, 2D transition metal carbides, and nitrides have attracted tremendous interest because of their metallic conductivity, solution processability, and excellent merits in energy storage and other applications. However, the pristine MXene films often suffer from poor ambient stability and mechanical properties that stem from their polar terminal groups and weak interlayer interactions. Here, a heteroatom doping strategy is developed to tailor the surface functionalities of MXene, followed by the addition of large-sized reduced graphene oxide (rGO) as conductive additives to achieve a scalable production of S, N-MXene/rGO (SNMG-40) hybrid film with high mechanical strength ( ≈ 45 MPa) and energy storage properties (698.5 F cm⁻³). Notably, the SNMG-40 film also demonstrates long-term cycling stability ( ≈ 98% capacitance retention after 30 000 cycles), which can be maintained under ambient condition or immersed in H₂SO₄ electrolyte for more than 100 days. The asymmetric supercapacitor (aMGSC) based on SNMG-40 film shows an ultrahigh energy density of 22.3 Wh kg⁻¹, which is much higher than those previously reported MXene-based materials. Moreover, the aMGSC also provides excellent mechanical durability under different deformation conditions. Thus, this strategy makes MXene materials more competitive for real-world applications such as flexible electronics and electromagnetic interference shielding.     

In Situ Induced Core–Shell Carbon-Encapsulated Amorphous Vanadium Oxide for Ultra-Long Cycle Life Aqueous Zinc-Ion Batteries

Inevitable dissolution in aqueous electrolytes, intrinsically low electrical conductivity, and sluggish reaction kinetics have significantly hampered the zinc storage performance of vanadium oxide-based cathode materials. Herein, core–shell N-doped carbon-encapsulated amorphous vanadium oxide arrays, prepared via a one-step nitridation process followed by in situ electrochemical induction, as a highly stable and efficient cathode material for aqueous zinc-ion batteries (AZIBs) are reported. In this design, the amorphous vanadium oxide core provides unobstructed ions diffusion routes and abundant active sites, while the N-doped carbon shell can ensure efficient electron transfer and greatly stabilize the vanadium oxide core. The assembled AZIBs exhibit remarkable discharge capacity (0.92 mAh cm⁻² at 0.5 mA cm⁻²), superior rate capability (0.51 mAh cm⁻² at 20 mA cm⁻²), and ultra-long cycling stability (≈100% capacity retention after 500 cycles at 0.5 mA cm⁻² and 97% capacity retention after 10 000 cycles at 20 mA cm⁻²). The working mechanism is further validated by in situ X-ray diffraction combined with ex situ tests. Moreover, the fabricated cathode is highly flexible, and the assembled quasi-solid-state AZIBs present stable electrochemical performance under large deformations. This work offers insights into the development of high-performance amorphous vanadium oxide-based cathodes for AZIBs.     

A Bioinspired Polymer-Based Composite Displaying Both Strong Adhesion and Anisotropic Thermal Conductivity

The integration and functionality of high-power electronic architectures or devices require a high strength and good heat flow at the interface. However, simultaneously improving the interfacial bonding and phonon transport of polymers is challenging because of the tradeoff between the cross-linked flexible chains and high-quality crystalline structure. Here, a copolymer, poly(dopamine methacrylate-co-hydroxyethyl methacrylate [P(DMA-HEMA)] is designed and synthesized, inspired by the snail and mussel adhesion. The copolymer achievs a high surface adhesion up to 6.38 MPa owing to the synergistic effects of hydrogen bonds and mechanical interlocking. When the copolymer is introduced into vertically aligned carbon nanotubes (VACNTs), the catechol groups in P(DMA-HEMA) formed strong bonding with the nanotubes through π-π interactions at the interface. As a result, the P(DMA-HEMA)/VACNTs composite shows a high through-plane thermal conductivity (21.46 W m⁻¹ K⁻¹), an in-plane thermal conductivity that is 3.5 times higher than that of pristine VACNTs, and an extremely low thermal contact resistance (20.27 K mm² W⁻¹). Furthermore, the composite forms weld-free high-strength connections between two pieces of various metals to bridge directional thermal pathways. It also exhibits excellent interfacial heat transfer capability and high reliability even under zero-pressure conditions.