Enhancing the Energy Storage Capabilities of Ti3C2Tx MXene Electrodes by Atomic Surface Reduction

MXenes are a large class of 2D materials that consist of few-atoms-thick layers of transition metal carbides, nitrides, or carbonitrides. The surface functionalization of MXenes has immense implications for their physical, chemical, and electronic properties. However, solution-phase surface functionalization often leads to structural degradation of the MXene electrodes. Here, a non-conventional, single-step atomic surface reduction (ASR) technique is adopted for the surface functionalization of MXene (Ti₃C₂T_x) in an atomic layer deposition reactor using trimethyl aluminum as a volatile reducing precursor. The chemical nature of the modified surface is characterized by X-ray photoelectron spectroscopy and nuclear magnetic resonance techniques. The electrochemical properties of the surface-modified MXene are evaluated in acidic and neutral aqueous electrolyte solutions, as well as in conventional Li-ion and Na-ion organic electrolytes. A considerable improvement in electrochemical performance is obtained for the treated electrodes in all the examined electrolyte solutions, expressed in superior rate capability and cycling stability compared to those of the non-treated MXene films. This improved electrochemical performance is attributed to the increased interlayer spacing and modified surface terminations after the ASR process.     

2D/2D 1T‐MoS2/Ti3C2 MXene Heterostructure with Excellent Supercapacitor Performance

2D/2D heterostructures can combine the collective advantages of each 2D material and even show improved properties from synergistic effects. 2D Transition metal carbide Ti₃C₂ MXene and 2D 1T‐MoS₂ have emerged as attractive prototypes in electrochemistry due to their rich properties. Construction of these two 2D materials, as well as investigation about synergistic effects, is absent due to the instability of 1T‐MoS₂. Here, 3D interconnected networks of 1T‐MoS₂/Ti₃C₂ MXene heterostructure are constructed by magneto‐hydrothermal synthesis, and the electrochemical storage mechanisms are investigated. Improved extra capacitance is observed due to enlarged ion storage space from a synergistically interplayed effect in 3D interconnected networks. Outstanding rate performance is realized because of ultrafast electron transport originating from Ti₃C₂ MXene. This work provides an archetype to realize excellent electrochemical properties in 2D/2D heterostructures.     

Strategy Toward Semiconducting Ti3C2Tx-MXene: Phenylsulfonic Acid Groups Modified Ti3C2Tx as Photosensitive Material for Flexible Visual Sensory-Neuromorphic System

The excellent electronic and electrochemical properties make 2D MXenes suitable candidates for sensors, batteries, and supercapacitors. However, the metallic-like behavior of MXenes hinders their potential for optoelectronic devices such as photodetectors. In this study, the band gap of metalloid Ti₃C₂T_x MXene is successfully opened to 1.53 eV with phenylsulfonic acid groups and realized a transistor and high-performance near-infrared photodetector array for a flexible vision sensory-neuromorphic system. The phenylsulfonic acid groups modified Ti₃C₂T_x MXene (S-Ti₃C₂T_x)-based flexible photodetector has a maximum responsivity of 8.50×10² A W⁻¹ and a detectivity of 3.69×10¹¹ Jones under 1064 nm laser irradiation. Moreover, the fabricated flexible vision sensory-neuromorphic system for image recognition realizes a high recognition rate >0.99, leading to great potential in the field of biological visual simulation and biomimetic eye. Besides conventional devices with Au as the conductive electrodes, all Ti₃C₂T_x MXene-based devices are also fabricated with S-Ti₃C₂T_x as the photosensitive material and unmodified Ti₃C₂T_x as the conductive electrodes, exhibiting comparable optoelectronic performances.     

Flexible Ti3C2Tx@Al electrodes with Ultrahigh Areal Capacitance: In Situ Regulation of Interlayer Conductivity and Spacing

Although Ti₃C₂ MXene has shown great potential in energy storage field, poor conductivity and restacking between MXene flakes seriously hinders the maximization of its capacitance. Herein, a new strategy to solve the problems is developed. Gallery Al atoms in Ti₃AlC₂ are partially removed by simple hydrothermal etching to get Ti₃C₂T_x reserving appropriate Al interlayers (Ti₃C₂T_x@Al). Ti₃C₂T_x@Al keeps stable layered structure rather than isolated Ti₃C₂T_x flakes, which avoids flake restacking. The removal of partial Al frees up space for easy electrolyte infiltration while the reserved Al as “electron bridges” ensures high interlayer conductivity. As a result, the areal capacitance reaches up to 1087 mF cm^?2 at 1 mA cm^?2 and over 95% capacitance is maintained after 6000 cycles. The all‐solid‐state supercapacitor (ASSS) based on Ti₃C₂T_x@Al delivers a high capacitance of 242.3 mF cm^?2 at 1 mV s^?1 and exhibits stable performance at different bending states. Two ASSSs in tandem can light up a light‐emitting diode under the planar or wrapping around an arm. The established strategy provides a new avenue to improve capacitance performances of MXenes.     

High-Performance Ultraviolet Photodetectors Enabled by van der Waals Schottky Junction Based on TiO2 Nanorod Arrays/Au-Modulated Ti3C2Tx MXene

Two-dimensional transition metal carbides and nitrides (MXenes) show tremendous potential for optoelectronic devices due to their excellent electronic properties. Here, a high-performance ultraviolet photodetector based on TiO₂ nanorod arrays/Ti₃C₂T_x MXene van der Waals (vdW) Schottky junction by all-solution process technique is reported. The Ti₃C₂T_x MXene modulated by the Au electrode increases its work function from 4.41 to 5.14 eV to form a hole transport layer. Complemented by the dangling bond-free surface of Ti₃C₂T_x, the Fermi-level pinning effect is suppressed and the electric-field strength of the Schottky junction is enhanced, which promotes charge separation and transport. After applying a bias of −1.5 V, the photovoltaic effect is favorably reinforced, while the hole-trapping mechanism (between TiO₂ and oxygen) and reverse pyroelectric effect are largely eliminated. As a result, the responsivity and specific detectivity of the device with FTO/TiO₂ nanorod arrays/Ti₃C₂T_x/Au structure reach 1.95 × 10⁵ mA W⁻¹ and 4.3 × 10¹³ cm Hz^1/2 W⁻¹ (370 nm, 65 mW cm⁻²), respectively. This work provides an effective approach to enhance the performance of photodetectors by forming the vdW Schottky junction and choosing metal electrodes to modulate MXene as a suitable charge transport layer.     

Tetrabutylammonium Bromide Functionalized Ti3C2Tx MXene as Versatile Cathode Buffer Layer for Efficient and Stable Inverted Perovskite Solar Cells

2D Ti₃C₂T_x MXene, possessing facile preparation, high electrical conductivity, flexibility, and solution processability, shows good application potential for enhancing device performance of perovskite solar cells (PVSCs). In this study, tetrabutylammonium bromide functionalized Ti₃C₂T_x (TBAB-Ti₃C₂T_x) is developed as cathode buffer layer (CBL) to regulate the PCBM/Ag cathode interfacial property for the first time. By virtue of the charge transfer from TBAB to Ti₃C₂T_x demonstrated by electron paramagnetic resonance and density functional theory, the TBAB-Ti₃C₂T_x CBL with high electrical conductivity exhibits significantly reduced work function of 3.9 eV, which enables optimization of energy level alignment and enhancement of charge extraction. Moreover, the TBAB-Ti₃C₂T_x CBL can effectively inhibit the migration of iodine ions from perovskite layer to Ag cathode, which synergistically suppresses defect states and reduce charge recombination. Consequently, utilizing MAPbI₃ perovskite without post-treatment, the TBAB-Ti₃C₂T_x based device exhibits a dramatically improved power conversion efficiency of 21.65% with significantly improved operational stability, which is one of the best efficiencies reported for the devices based on MAPbI₃/PCBM with different CBLs. These results indicate that TBAB-Ti₃C₂T_x shall be a promising CBL for high-performance inverted PVSCs and inspire the further applications of quaternary ammonium functionalized MXenes in PVSCs.     

Tailoring Ultrahigh Energy Density and Stable Dendrite-Free Flexible Anode with Ti3C2Tx MXene Nanosheets and Hydrated Ammonium Vanadate Nanobelts for Aqueous Rocking-Chair Zinc Ion Batteries

Exploiting Zn metal-free anode materials would be an effective strategy to resolve the problems of Zn metal dendrites that severely hinder the development of Zn ion batteries (ZIBs). However, the study of Zn metal-free anode materials is still in their infancy, and more importantly, the low energy density severely limits their practical implementations. Herein, a novel (NH₄)₂V₁₀O₂₅ · 8H₂O@Ti₃C₂T_x (NHVO@Ti₃C₂T_x) film anode is proposed and investigated for constructing “rocking-chair” ZIBs. The NHVO@Ti₃C₂T_x electrode shows a capacity of 514.7 mAh g⁻¹ and presents low potential which is 0.59 V (vs Zn²⁺/Zn) at 0.1 A g⁻¹. The introduction of Ti₃C₂T_x not only affords an interconnected conductive network, but also stabilizes the NHVO nanobelts structure for a long cycle life (84.2% retention at 5.0 A g⁻¹ over 6000 cycles). As a proof-of-concept, a zinc metal-free full battery is successfully demonstrated, which delivers the highest capacity of 131.7 mAh g⁻¹ (mass containing anodic and cathodic) and energy density of 97.1 Wh kg⁻¹ compared to all reported aqueous “rocking-chair” ZIBs. Furthermore, a long cycling span of 6000 cycles is obtained with capacity retention reaching up to 92.1%, which is impressive. This work is expected to provide new moment toward V-based materials for “rocking-chair” ZIBs.     

Enhancing the Capacitive Storage Performance of Carbon Fiber Textile by Surface and Structural Modulation for Advanced Flexible Asymmetric Supercapacitors

The exploration of high‐energy anodes with good mechanical properties is highly attractive for flexible asymmetric supercapacitors (ASCs) but challenging. Owing to the excellent conductivity and superior mechanical flexibility, carbon fiber textile (CFT) holds great promise as a substrate/current‐collector for fabricating flexible electrodes. Yet, it is rarely used as a flexible active electrode in terms of its low electrochemical reactivity and small accessible area. In this work, an effective surface and structural modulation strategy is developed to directly tune CFT into a highly active anode for flexible ASCs by creating hierarchical pores and numerous pseudocapacitive oxygenic groups. Arising from large surface and increased active sites, the as‐prepared activated porous CFT (APCFT) electrode not only achieves a large capacitance (1.2 F cm^?2 at 4 mA cm^?2) and fast kinetics but also shows satisfying cycling durability (no capacitance decay after 25 000 cycles). More importantly, an advanced flexible ASC device with an impressive energy density of 4.70 mWh cm^?3 is successfully assembled by employing this APCFT as an anode, outperforming most recently reported ASC devices. This dual modification strategy may throw light on the rational design of new generation advanced carbon electrodes for high‐performance flexible supercapacitors.     

Removal of Interlayer Water of two Ti3C2Tx MXenes as a Versatile Tool for Controlling the Fermi-Level Pinning-Free Schottky Diodes with Nb:SrTiO3

Striving for the sixth-generation communication technology discovery, semiconductors beyond Si with wider bandgaps as well as non-conventional metals are actively being sought to achieve high speeds whilst maintaining devices miniaturization. 2D materials may provide the potential for downsizing, but their functional advantage over existing counterparts still longs to be discovered. Along that path, surface-adsorbed or bulk-intercalated water molecules remaining after wet-chemical synthesis of 2D materials are generally seen as obstacles to high-performance achievement. Herein, the control of such water within the interlayers of solution-processed metallic 2D titanium carbide (MXene) by vacuum annealing duration is demonstrated. Moreover, the impact of water removal on work function (WF) and functional terminations is unveiled for the first time. Furthermore, the usefulness of such water for controlling a novel Schottky diode in contact with an n-type oxide semiconductor, niobium-doped strontium titanate (Nb:SrTiO₃) is observed. The advantage of MXene compared to conventional gold as facile processing, WF tunability, and lower turn-on voltage in the Schottky anode application is highlighted. This fundamental study shows the way for a novel Schottky diode preparation in atmospheric conditions and provides implications for further research directions aiming at commercialization.     

Oxygen Vacancies Modified TiO2/O-Terminated Ti3C2 Composites: Unravelling the Dual Effects between Oxygen Vacancy and High-Work-Function Titanium Carbide

The rational design of Ti₃C₂T_x MXene-derived TiO₂-based photocatalysts with broad light absorption and efficient charge separation has recently attracted considerable attention for antibiotic degradation. However, the complementary effects of each component, especially oxygen vacancies (OVs) and high work function O-terminated Ti₃C₂ (O-Ti₃C₂), in affecting light absorption and photocatalytic activity remain controversial. In this study, Ti₃C₂T_x-derived TiO₂/Ti₃C₂T_x photocatalysts are regulated by alkalization in the controlled KOH solution and calcination in different heating atmospheres to reveal the contribution of OVs, Ti³⁺, carbon species, and high work function titanium carbide. Carbon species and rich OVs co-exist in TiO₂/O-Ti₃C₂ (OV/C-TT-1K(N₂)) which exhibit superior photocatalytic performance in tetracycline hydrochloride degradation with a kinetic constant of 0.0217 min⁻¹. Combined with experimental and DFT computational results, the broadened visible light response and desirable redox properties are caused by OVs and carbon dopants, as well as decreased Schottky barrier height and enhanced electronic conductivity caused by high work function O-Ti₃C₂.     

Surface‐Modified Metallic Ti3C2Tx MXene as Electron Transport Layer for Planar Heterojunction Perovskite Solar Cells

MXenes are a large and rapidly expanding family of 2D materials that, owing to their unique optoelectronic properties and tunable surface termination, find a wide range of applications including energy storage and energy conversion. In this work, Ti₃C₂T_x MXene nanosheets are applied as a novel type of electron transport layer (ETL) in low‐temperature processed planar‐structured perovskite solar cells (PSCs). Interestingly, simple UV‐ozone treatment of the metallic Ti₃C₂T_x that increases the surface Ti? O bonds without any change in its bulk properties such as high electron mobility improves its suitability as an ETL. Improved electron transfer and suppressed recombination at the ETL/perovskite interface results in augmentation of the power conversion efficiency (PCE) from 5.00% in the case of Ti₃C₂T_x without UV‐ozone treatment to the champion PCE of 17.17%, achieved using the Ti₃C₂T_x film after 30 min of UV‐ozone treatment. As the first report on the use of pure MXene layer as an ETL in PSCs, this work shows the great potential of MXenes to be used in PSCs and displays their promise for applications in photovoltaic technology in general.     

High Linearity,Low Hysteresis Ti3C2Tx MXene/AgNW/Liquid Metal Self-Healing Strain Sensor Modulated by Dynamic Disulfide and Hydrogen Bonds

Flexible wearable strain sensors have received extensive attention in human–computer interaction, soft robotics, and human health monitoring. Despite significant efforts in developing stretchable electronic materials and structures, developing flexible strain sensors with stable interfaces and low hysteresis remains a challenge. Herein, Ti₃C₂T_x MXene/AgNWs/liquid metal strain sensors (MAL strain sensor) with self-healing function are developed by exploiting the strong interactions between Ti₃C₂T_x MXene/AgNWs/LM and the disulfide and hydrogen bonds inside the self-healing poly(dimethylsiloxane) elastomers. AgNWs lap the Ti₃C₂T_x MXene sheets, and the LM acts as a bridge to increase the lap between Ti₃C₂T_x MXene and AgNWs, thereby improving the interface interaction between them and reducing hysteresis. The MAL strain sensor can simultaneously achieve high sensitivity (gauge factor for up to 3.22), high linearity (R² = 0.98157), a wide range of detection (e.g., 1%–300%), a fast response time (145 ms), excellent repeatability, and stability.In addition, the MAL strain sensor before and after self-healing is combined with a small fish and an electrothermally driven soft robot, respectively, allowing real-time monitoring of the swinging tail of the small fish and the crawling of the soft robot by resistance changes.     

Strain Sensors with a High Sensitivity and a Wide Sensing Range Based on a Ti3C2Tx (MXene) Nanoparticle–Nanosheet Hybrid Network

A high sensitivity and large stretchability are desirable for strain sensors in wearable applications. However, these two performance indicators are contradictory, since the former requires a conspicuous structural change under a tiny strain, whereas the latter demands morphological integrity upon a large deformation. Developing strain sensors with both a high sensitivity (gauge factor (GF) > 100) and a broad strain range (>50%) is a considerable challenge. Herein, a unique Ti₃C₂T_x MXene nanoparticle–nanosheet hybrid network is constructed. The migration of nanoparticles leads to a large resistance variation while the wrapping of nanosheet bridges the detached nanoparticles to maintain the connectivity of the conductive pathways in a large strain region. The synergetic motion of nanoparticles and nanosheets endows the hybrid network with splendid electrical–mechanical performance, which is reflected in its high sensitivity (GF > 178.4) over the entire broad range (53%), the super low detection limit (0.025%), and a good cycling durability (over 5000 cycles). Such high performance endows the strain sensor with the capability for full‐range human motion detection.     

Controllable Patterning of Porous MXene (Ti3C2) by Metal-Assisted Electro-Gelation Method

Since discovered in 2011, transition metal carbides or nitrides (MXenes) have attracted enormous attention due to their unique properties. Morphology regulation strategies assembling 2D MXene sheets into 3D architecture have endowed the as-formed porous MXene with a better performance in various fields. However, the direct patterning strategy for the porous MXene into integration with multifunctional and multichannel electronic devices still needs to be investigated. The metal-assisted electro-gelation method the authors propose can directly generate porous-structured MXene hydrogel with a tunable feature. By electrolyzing the sacrificial metal, the released metal cations initiate the electro-gelation process during which electrostatic interactions occur between cations and the MXene sheets. A high spatial resolution down to micro-meter level is achieved utilizing the method, enabling high-performance hydrogels with more complex architectures. Electronics prepared through this metal-assisted electro-gelation process have shown promising applications of the porous MXene in energy and biochemical sensing fields. Energy storage devices with a capacitance at 33.3 mF cm⁻² and biochemical sensors show prominent current responses towards metabolites (sensitivity of H₂O₂: 165.6  µ A mm ⁻¹ cm⁻²; sensitivity of DA: 212 nA  µ m ⁻¹ cm⁻²), suggesting that the metal-assisted electro-gelation method will become a prospective technique for advanced fabrication of MXene-based devices.     

Tuning Thermal Transport Through Atomically Thin Ti3C2Tz MXene by Current Annealing in Vacuum

Heat transport across vertical interfaces of heterogeneous 2D materials is usually governed by the weak Van der Waals interactions of the surface‐terminating atoms. Such interactions play a significant role in thermal transport across transition metal carbide and nitride (MXene) atomic layers due to their hydrophilic nature and variations in surface terminations. Here, the metallicity of atomically thin Ti₃C₂T_z MXene, which is also verified by scanning tunneling spectroscopy for the first time, is exploited to develop a self‐heating/self‐sensing platform to carry out direct‐current annealing experiments in high (<10^?8 bar) vacuum, while simultaneously evaluating the interfacial heat transport across a Ti₃C₂T_z/SiO₂ interface. At room temperature, the thermal boundary conductance (TBC) of this interface is found, on average, to increase from 10 to 27 MW m^?2 K^?1 upon current annealing up to the breakdown limit. In situ heating X‐ray diffraction and X‐ray photo‐electron spectroscopy reveal that the TBC values are mainly affected by interlayer and interface spacing due to the removal of absorbents, while the effect of surface termination is negligible. This study provides key insights into understanding energy transport in MXene nanostructures and other 2D material systems.     

Ti：Al_2O_3晶体荧光浓度猝灭及其能量转移机理

根据Ｄｅｘｔｅｒ敏化发光理论建立Ｔｉ３＋－Ｔｉ３＋离子间能量共振转移模型，计算出Ｔｉ：Ａｌ２Ｏ３晶体发生浓度猝灭的Ｔｉ３＋离子临界距离Ｒｃ及晶体掺杂的临界浓度Ｎｃ与实测光谱数据进行比较，认为浓度达到Ｎ＝１．２８×１０２０ｃｍ－３（或０．３８ｗｔ％），相应峰值吸收系数为α４９０＝６．０ｃｍ－１时，仍未发生明显的浓度猝灭现象。     

Atomic Sulfur Covalently Engineered Interlayers of Ti3C2 MXene for Ultra‐Fast Sodium‐Ion Storage by Enhanced Pseudocapacitance

2D MXenes have been widely applied in the field of electrochemical energy storage owning to their high electrical conductivity and large redox‐active surface area. However, electrodes made from multilayered MXene with small interlayer spacing exhibit sluggish kinetics with low capacity for sodium‐ion storage. Herein, Ti₃C₂ MXene with expanded and engineered interlayer spacing for excellent storage capability is demonstrated. After cetyltrimethylammonium bromide pretreatment, S atoms are successfully intercalated into the interlayer of Ti₃C₂ to form a desirable interlayer‐expanded structure via Ti? S bonding, while pristine Ti₃C₂ is hardly to be intercalated. When the annealing temperature is 450 °C, the S atoms intercalated Ti₃C₂ (CT‐S@Ti₃C₂‐450) electrode delivers the improved Na‐ion capacity of 550 mAh g^?1 at 0.1 A g^?1 (≈120 mAh g^?1 at 15 A g^?1, the best MXene‐based Na⁺‐storage rate performance reported so far), and excellent cycling stability over 5000 cycles at 10 A g^?1 by enhanced pseudocapacitance. The enhanced sodium‐ion storage capability has also been verified by theoretical calculations and kinetic analysis. Coupling the CT‐S@Ti₃C₂‐450 anode with commercial AC cathode, the assembled Na⁺ capacitor delivers high energy density (263.2 Wh kg^?1) under high power density (8240 W kg^?1), and outstanding cycling performance.     

Integrated Quasiplane Heteronanostructures of MoSe2/Bi2Se3 Hexagonal Nanosheets: Synergetic Electrocatalytic Water Splitting and Enhanced Supercapacitor Performance

MoSe₂ as a typical transition metal dichalcogenide holds great potential for energy storage and catalysis but its performance is largely limited by its poor conductivity. Bi₂Se₃ nanosheets, a kind of topological insulators, possess gapless edges on boundary and show metallic character on surface. According to the principle of complementary, a novel integrated quasiplane structure of MoSe₂/Bi₂Se₃ hybrids is designed with artistic heteronanostructures via a hot injection in colloidal system. Interestingly, the heteronanostructures are typically constituted by single‐layer Bi₂Se₃ hexagonal nanoplates evenly enclosed by small ultrathin hierarchical MoSe₂ nanosheets on the whole surfaces. X‐ray photoelectron spectroscopy investigations suggest obvious electron transfer from Bi₂Se₃ to MoSe₂, which can help to enhance the conductivity of the hybrid electrode. Especially, schematic energy band diagrams derived from ultraviolet photoelectron spectroscopy studies indicate that Bi₂Se₃ has higher E_F and smaller Φ than MoSe₂, further confirming the electronic modulation between Bi₂Se₃ and MoSe₂, where Bi₂Se₃ serves as an excellent substrate to provide electrons and acts as channels for high‐rate transition. The MoSe₂/Bi₂Se₃ hybrids demonstrating a low onset potential, small Tafel slope, high current density, and long‐term stability suggest excellent hydrogen evolution reaction activity, whereas a high specific capacitance, satisfactory rate capability, and rapid ions diffusion indicate enhanced supercapacitor performance.     

Electrical properties of Ge metal–oxide–semiconductor capacitors with high-k La2O3 gate dielectric incorporated by N or/and Ti

LaON, LaTiO and LaTiON films are deposited as gate dielectrics by incorporating N or/and Ti into La2O3 using the sputtering method to fabricate Ge MOS capacitors, and the electrical properties of the devices are carefully examined. LaON/Ge capacitors exhibit the best interface quality, gate leakage property and device reliability, but a smaller k value (14.9). LaTiO/Ge capacitors exhibit a higher k value (22.7), but a deteriorated interface quality, gate leakage property and device reliability. LaTiON/Ge capacitors exhibit the highest k value (24.6), and a relatively better interface quality (3.1E11 eV^-1cm^-2), gate leakage property (3.6E3 A/cm^2 at Vg = 1 V + Vfb) and device reliability. Therefore, LaTiON is more suitable for high performance Ge MOS devices as a gate dielectric than LaON and LaTiO materials.     

Achieving of Flexible,Free‐Standing,Ultracompact Delaminated Titanium Carbide Films for High Volumetric Performance and Heat‐Resistant Symmetric Supercapacitors

The volumetric performance of supercapacitors (SCs), besides the gravimetric performance, is attracting an increasing attention due to the fast development of electric vehicles and smart devices. Here, a unique design of symmetric supercapacitor material is reported with a tight face‐to‐face architecture by applying a high pressure to the delaminated Ti₃C₂ (d‐Ti₃C₂) films. The high pressure makes the d‐Ti₃C₂ films achieve an increased density, high electron conductivity, good wettability, and abundant interconnected mesopore channels to promote ion transport efficiently, that is, more cations can intercalate/deintercalate in the charging–discharging process. As a result, with the increase of the applying pressure, the d‐Ti₃C₂ film pressured at 40 MPa in 1 m Li₂SO₄ exhibits an ultrahigh capacitance of over 633 F cm^?3, outstanding energy density, and cyclic stability. Especially, the corresponding SC in 1 m 1‐ethyl‐3‐methylimidazolium tetrafluoroborate/acetonitrile organic electrolyte shows a high volumetric energy density of 41 Wh L^?1, which is the highest value reported for the SCs based on MXene materials in organic electrolytes. The outstanding volumetric electrochemical performance and thermal stability of the SCs based on the ultracompact d‐Ti₃C₂ film demonstrate their promising potential as forceful power sources for small electronic devices.