A Flexible 3D Multifunctional MgO‐Decorated Carbon Foam@CNTs Hybrid as Self‐Supported Cathode for High‐Performance Lithium‐Sulfur Batteries

One of the critical challenges to develop advanced lithium‐sulfur (Li‐S) batteries lies in exploring a high efficient stable sulfur cathode with robust conductive framework and high sulfur loading. Herein, a 3D flexible multifunctional hybrid is rationally constructed consisting of nitrogen‐doped carbon foam@CNTs decorated with ultrafine MgO nanoparticles for the use as advanced current collector. The dense carbon nanotubes uniformly wrapped on the carbon foam skeletons enhance the flexibility and build an interconnected conductive network for rapid ionic/electronic transport. In particular, a synergistic action of MgO nanoparticles and in situ N‐doping significantly suppresses the shuttling effect via enhanced chemisorption of lithium polysulfides. Owing to these merits, the as‐built electrode with an ultrahigh sulfur loading of 14.4 mg cm^?2 manifests a high initial areal capacity of 10.4 mAh cm^?2, still retains 8.8 mAh cm^?2 (612 mAh g^?1 in gravimetric capacity) over 50 cycles. The best cycling performance is achieved upon 800 cycles with an extremely low decay rate of 0.06% at 2 C. Furthermore, a flexible soft‐packaged Li‐S battery is readily assembled, which highlights stable electrochemical characteristics under bending and even folding. This cathode structural design may open up a potential avenue for practical application of high‐sulfur‐loading Li‐S batteries toward flexible energy‐storage devices.     

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.     

A Printable Metallic Current Collector for All‐Printed High‐Voltage Micro‐Supercapacitors: Instantaneous Surface Passivation by Flash‐Light‐Sintering Reaction

Recently, a printable power source that can be implemented on demand in integrated circuitries has gained tremendous attention to facilitate next‐generation, form‐factor free, miniaturized electronic systems. Among various energy storage units, a solid‐state micro‐supercapacitor with in‐plane device architecture has been recognized as a viable candidate with characteristic advantages of long cycle life‐time, high frequency response, and fast charge/discharge rate. However, to date, high performance, all‐printed micro‐supercapacitors have rarely been reported owing to an absence of printable current collector materials that can sustain high voltage conditions. In this study, a multidimensional printable particle mixture comprising Ni nanoparticles, Ni flakes, and a photoreactive polymer, polyvinylpyrrolidone is proposed. The highly conductive, printed metallic current collector is generated with a conductive surface passivation layer in a timescale of 10^?3 s by flash‐light sintering process. It is revealed that the resulting metallic current collector is stable at a voltage as high as 3 V in the carbon electrode‐based device, enabling the fabrication of an all‐printed solid‐state micro‐supercapacitor with an areal energy density of 79–23 mJ cm^?2 at an areal power density of 0.4–12.8 mW cm^?2. Arbitrarily designed device circuits can be generated on demand simply by using a digitally programmable printing process, without incorporation of additional interconnection lines.     

Wood‐Inspired Morphologically Tunable Aligned Hydrogel for High‐Performance Flexible All‐Solid‐State Supercapacitors

Oriented microstructures are widely found in various biological systems for multiple functions. Such anisotropic structures provide low tortuosity and sufficient surface area, desirable for the design of high‐performance energy storage devices. Despite significant efforts to develop supercapacitors with aligned morphology, challenges remain due to the predefined pore sizes, limited mechanical flexibility, and low mass loading. Herein, a wood‐inspired flexible all‐solid‐state hydrogel supercapacitor is demonstrated by morphologically tuning the aligned hydrogel matrix toward high electrode‐materials loading and high areal capacitance. The highly aligned matrix exhibits broad morphological tunability (47–12 µm), mechanical flexibility (0°–180° bending), and uniform polypyrrole loading up to 7 mm thick matrix. After being assembled into a solid‐state supercapacitor, the areal capacitance reaches 831 mF cm^?2 for the 12 µm matrix, which is 259% times of the 47 µm matrix and 403% times of nonaligned matrix. The supercapacitor also exhibits a high energy density of 73.8 µWh cm^?2, power density of 4960 µW cm^?2, capacitance retention of 86.5% after 1000 cycles, and bending stability of 95% after 5000 cycles. The principle to structurally design the oriented matrices for high electrode material loading opens up the possibility for advanced energy storage applications.     

Vertically Aligned Carbon Nanofibers on Cu Foil as a 3D Current Collector for Reversible Li Plating/Stripping toward High‐Performance Li–S Batteries

A vertically aligned carbon nanofiber (VACNF) array with unique conically stacked graphitic structure directly grown on a planar Cu current collector (denoted as VACNF/Cu) is used as a high‐porosity 3D host to overcome the commonly encountered issues of Li metal anodes. The excellent electrical conductivity and highly active lithiophilic graphitic edge sites facilitate homogenous coaxial Li plating/stripping around each VACNF and forming a uniform solid electrolyte interphase. The high specific surface area effectively reduces the local current density and suppresses dendrite growth during the charging/discharging processes. Meanwhile, this open nanoscale vertical 3D structure eliminates the volume changes during Li plating/stripping. As a result, highly reversible Li plating/stripping with high coulombic efficiency is achieved at various current densities. A low voltage hysteresis of 35 mV over 500 h in symmetric cells is achieved at 1 mA cm^?2 with an areal Li plating capacity of 2 mAh cm^?2, which is far superior to the planar Cu current collector. Furthermore, a Li–S battery using a S@PAN cathode and a lithium‐plated VACNF/Cu (VACNF/Cu@Li) anode with slightly higher capacity (2 mAh cm^?2) exhibits an excellent rate capability and high cycling stability with no capacity fading over 600 cycles.     

A High Energy Density Asymmetric Supercapacitor from Nano‐architectured Ni(OH)2/Carbon Nanotube Electrodes

The demand for advanced energy storage devices such as supercapacitors and lithium‐ion batteries has been increasing to meet the application requirements of hybrid vehicles and renewable energy systems. A major limitation of state‐of‐art supercapacitors lies in their relatively low energy density compared with lithium batteries although they have superior power density and cycle life. Here, we report an additive‐free, nano‐architectured nickel hydroxide/carbon nanotube (Ni(OH)₂/CNT) electrode for high energy density supercapacitors prepared by a facile two‐step fabrication method. This Ni(OH)₂/CNT electrode consists of a thick layer of conformable Ni(OH)₂ nano‐flakes on CNT bundles directly grown on Ni foams (NFs) with a very high areal mass loading of 4.85 mg cm^?2 for Ni(OH)₂. Our Ni(OH)₂/CNT/NF electrode demonstrates the highest specific capacitance of 3300 F g^?1 and highest areal capacitance of 16 F cm^?2, to the best of our knowledge. An asymmetric supercapacitor using the Ni(OH)₂/CNT/NF electrode as the anode assembled with an activated carbon (AC) cathode can achieve a high cell voltage of 1.8 V and an energy density up to 50.6 Wh/kg, over 10 times higher than that of traditional electrochemical double‐layer capacitors (EDLCs).     

Engineering 3D Ion Transport Channels for Flexible MXene Films with Superior Capacitive Performance

2D MXene materials are of considerable interest for future energy storage. A MXene film could be used as an effective flexible supercapacitor electrode due to its flexibility and, more importantly, its high specific capacitance. However, although it has excellent electronic conductivity, sluggish ionic kinetics within the MXene film becomes a fundamental limitation to the electrochemical performance. To compensate for the relative deficiency, MXene films are frequently reduced to several micrometer dimensions with low mass loading (<1 mg cm^?2), to the point of detriment of areal performance and commercial value. Herein, for the first time, the design of a 3D porous MXene/bacterial cellulose (BC) self‐supporting film is reported for ultrahigh capacitance performance (416 F g^?1, 2084 mF cm^?2) with outstanding mechanical properties and high flexibility, even when the MXene loading reaches 5 mg cm^?2. The highly interconnected MXene/BC network enables both excellent electron and ion transport channel. Additionally, a maximum energy density of 252 µWh cm^?2 is achieved in an asymmetric supercapacitor, higher than that of all ever‐reported MXene‐based supercapacitors. This work exploits a simple route for assembling 2D MXene materials into 3D porous films as state‐of‐the‐art electrodes for high performance energy storage devices.     

A Low‐Cost,Self‐Standing NiCo2O4@CNT/CNT Multilayer Electrode for Flexible Asymmetric Solid‐State Supercapacitors

The demand for a new generation of flexible, portable, and high‐capacity power sources increases rapidly with the development of advanced wearable electronic devices. Here we report a simple process for large‐scale fabrication of self‐standing composite film electrodes composed of NiCo₂O₄@carbon nanotube (CNT) for supercapacitors. Among all composite electrodes prepared, the one fired in air displays the best electrochemical behavior, achieving a specific capacitance of 1,590 F g^?1 at 0.5 A g^?1 while maintaining excellent stability. The NiCo₂O₄@CNT/CNT film electrodes are fabricated via stacking NiCo₂O₄@CNT and CNT alternately through vacuum filtration. Lightweight, flexible, and self‐standing film electrodes (≈24.3 µm thick) exhibit high volumetric capacitance of 873 F cm^?3 (with an areal mass of 2.5 mg cm^?2) at 0.5 A g^?1. An all‐solid‐state asymmetric supercapacitor consists of a composite film electrode and a treated carbon cloth electrode has not only high energy density (≈27.6 Wh kg^?1) at 0.55 kW kg^?1 (including the weight of the two electrodes) but also excellent cycling stability (retaining ≈95% of the initial capacitance after 5000 cycles), demonstrating the potential for practical application in wearable devices.     

Development of Graphene Oxide/Polyaniline Inks for High Performance Flexible Microsupercapacitors via Extrusion Printing

Extrusion printing of interdigitated electrodes for flexible microsupercapacitors (fMSCs) offers an attractive route to the fabrication of flexible devices where cost, scalability, and processability of ink formulations are critical. In this work, highly concentrated, viscous, and water‐dispersible inks are developed based on graphene oxide (GO)/polyaniline (PANi) composite for extrusion printing. The optimized GO/PANi‐based all‐solid‐state symmetric fMSCs obtained by extrusion printing interdigitated microelectrodes can deliver outstanding areal capacitance of 153.6 mF cm^?2 and volumetric capacitance of 19.2 F cm^?3 at 5 mV s^?1. It is shown that by fabricating asymmetric fMSCs using the GO/PANi as positive electrode and a graphene‐based negative electrode, the voltage window can be widened from 0.8 to 1.2 V and improvements can be achieved in energy density (from 3.36 to 4.83 mWh cm^?3), power density (from 9.82 to 25.3 W cm^?3), and cycling stability (from 75% to 100% capacitance retention over 5000 cycles) compared with the symmetric counterpart. The simple ink preparation and facile device fabrication protocols reported here make the scalable fabrication of extrusion printed fMSCs a promising technology.     

Oxygen‐Deficient Bismuth Oxide/Graphene of Ultrahigh Capacitance as Advanced Flexible Anode for Asymmetric Supercapacitors

Oxygen‐deficient bismuth oxide (r‐Bi₂O₃)/graphene (GN) is designed, fabricated, and demonstrated via a facile solvothermal and subsequent solution reduction method. The ultrafine network bacterial cellulose (BC) as substrate for r‐Bi₂O₃/GN exhibits high flexibility, remarkable tensile strength (55.1 MPa), and large mass loading of 9.8 mg cm^?2. The flexible r‐Bi₂O₃/GN/BC anode delivers appreciable areal capacitance (6675 mF cm^?2 at 1 mA cm^?2) coupled with good rate capability (3750 mF cm^?2 at 50 mA cm^?2). In addition, oxygen vacancies have great influence on the capacitive performance of Bi₂O₃, delivering significantly improved capacitive values than the untreated Bi₂O₃ flexible electrode, and ultrahigh gravimetric capacitance of 1137 F g^?1 (based on the mass of r‐Bi₂O₃) can be obtained, achieving 83% of the theoretical value (1370 F g^?1). Flexible asymmetric supercapacitor is fabricated with r‐Bi₂O₃/GN/BC and Co₃O₄/GN/BC paper as the negative and positive electrodes, respectively. The operation voltage is expanded to 1.6 V, revealing a maximum areal energy density of 0.449 mWh cm^?2 (7.74 mWh cm^?3) and an areal power density of 40 mW cm^?2 (690 mW cm^?3). Therefore, this flexible anode with excellent electrochemical performance and high mechanical properties shows great potential in the field of flexible energy storage devices.     

Fabrication of Highly Flexible,Scalable, and High‐Performance Supercapacitors Using Polyaniline/Reduced Graphene Oxide Film with Enhanced Electrical Conductivity and Crystallinity

With developments in technology, tremendous effort has been devoted to produce flexible, scalable, and high‐performance supercapacitor electrode materials. This report presents a novel fabrication method of highly flexible and scalable electrode material for high‐performance supercapacitors using solution‐processed polyaniline (PANI)/reduced graphene oxide (RGO) hybrid film. SEM, TEM, Raman, and XPS analyses show that the PANI/RGO film is successfully synthesized. The percentages of the PANI component in the film are controlled (88, 76, and 60%), and the maximum electrical conductivity (906 S cm^?1) is observed at the PANI percentage of 76%. Notably, electrical conductivity of the PANI/RGO film (906 S cm^?1) is larger than both PANI (580 S cm^?1) and RGO (46.5 S cm^?1) components. XRD analysis demonstrates that the strong π–π interaction between the RGO and the PANI cause more compact packing of the PANI chains by inducing more fully expanded conformation of the PANI chains in the solution, leading to increase in the electrical conductivity and crystallinity of the film. The PANI/RGO film also displays diverse advantages as a scalable and flexible electrode material (e.g., controllable size and great flexibility). During the electrochemical tests, the film exhibits high capacitance of 431 F g^?1 with enhanced cycling stability.     

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.     

Hierarchical Free‐Standing Carbon‐Nanotube Paper Electrodes with Ultrahigh Sulfur‐Loading for Lithium–Sulfur Batteries

The rational combination of conductive nanocarbon with sulfur leads to the formation of composite cathodes that can take full advantage of each building block; this is an effective way to construct cathode materials for lithium–sulfur (Li–S) batteries with high energy density. Generally, the areal sulfur‐loading amount is less than 2.0 mg cm^?2, resulting in a low areal capacity far below the acceptable value for practical applications. In this contribution, a hierarchical free‐standing carbon nanotube (CNT)‐S paper electrode with an ultrahigh sulfur‐loading of 6.3 mg cm^?2 is fabricated using a facile bottom–up strategy. In the CNT–S paper electrode, short multi‐walled CNTs are employed as the short‐range electrical conductive framework for sulfur accommodation, while the super‐long CNTs serve as both the long‐range conductive network and the intercrossed mechanical scaffold. An initial discharge capacity of 6.2 mA·h cm^?2 (995 mA·h g^?1), a 60% utilization of sulfur, and a slow cyclic fading rate of 0.20%/cycle within the initial 150 cycles at a low current density of 0.05 C are achieved. The areal capacity can be further increased to 15.1 mA·h cm^?2 by stacking three CNT–S paper electrodes—resulting in an areal sulfur‐loading of 17.3 mg cm^?2—for the cathode of a Li–S cell. The as‐obtained free‐standing paper electrode are of low cost and provide high energy density, making them promising for flexible electronic devices based on Li–S batteries.     

Nature-Inspired Interconnected Macro/Meso/Micro-Porous MXene Electrode

The geometric multiplication development of MXene has promoted it to become a star material in numerous applications including, but not limited to, energy storage. It is found that pore structure modulation engineering can improve the inherent properties of MXene, in turn significantly enhancing its electrochemical performance. However, most of the current works have focused on exploring the structure-effective relationships of the single-scale pore structure regulation of MXene. Inspired by Murray's law from nature where a highly graded structure of the organisms is discovered and used to achieve effective diffusion and maximize mass transfer, a hierarchically interconnected porous MXene electrode across micro-meso-macroporous is constructed. This MXene-based electrode provides large amounts of active sites while greatly shortening the ion diffusion channel. Finally, the zinc ion microcapacitor based on this MXene electrode exhibits an ultrahigh area-specific capacitance up to 410 mF cm⁻² and an energy density up to 103 µWh cm⁻² at a power density of 2100 µW cm⁻². The areal energy density outperforms the currently reported zinc ion microcapacitors. This study supports an effective strategy for electrode materials (including but not limited to MXene) to achieve ultra-short ion diffusion channels and maximum transport efficiency for next-generation high-performance energy storage.     

Ultrahigh‐Strength Ultrahigh Molecular Weight Polyethylene (UHMWPE)‐Based Fiber Electrode for High Performance Flexible Supercapacitors

Flexible fiber‐based supercapacitor (FSC) with excellent electrochemical performance and high tensile strength and modulus is strongly desired for some special circumstances, such as load‐bearing, abrasion resistant, and anticutting fabrics. Here, a series of ultrahigh‐strength fiber electrodes are prepared for flexible FSCs based on ultrahigh molecular weight polyethylene fibers, on which the polydopamine, Ag, and poly (3,4‐ethylene dioxythiophene): poly(styrenesulfonate) are deposited in sequence. The modified fiber‐based electrode exhibits superhigh strength up to 3.72 GPa, which is the highest among fiber‐based electrodes reported to date. In addition, FSCs fabricated with the optimized fiber electrode shows a specific areal capacity as high as 563 mF cm^?2 at 0.17 mA cm^?2, which corresponds to a high areal energy density of ≈50.1 µWh cm^?2 at a power density of ≈124 µW cm^?2. The specific areal capacity only decrease 8% after 1000 times bending test, indicating the outstanding bending performance of this composite fiber electrode. Furthermore, several FSCs can be connected in series or in parallel to get higher working voltage or higher capacity respectively, which demonstrates its potential for broad applications in flexible devices.     

Sustainable 3D Structural Binder for High-Performance Supercapacitor by Biosynthesis Process

Flexible supercapacitors represent an attractive technology for the next generation of wearable consumer electronics as power sources but usually suffer from relatively low energy density. It is highly desired to construct high-performance electrodes for the practical applications of supercapacitors. Here, inspired by the natural structure of the spider web, an elaborate design of binder is reported through a biosynthesis process to construct flexible electrodes with both excellent mechanical properties and electrochemical performance. Through this strategy, a spider-web-inspired 3D structural binder enables large ion-accessible surface area and high packing density of active electrode material as well as efficient ion transport pathways. As a result, a high areal capacitance of 4.62 F cm^-2 and a high areal energy density of 0.18 mW h cm^-2 is achieved in the composite electrodes and symmetric supercapacitors, respectively, demonstrating a promising potential to construct flexible energy storage devices for diverse practical applications.     

Silicon Nanofibrils on a Flexible Current Collector for Bendable Lithium‐Ion Battery Anodes

A high‐energy‐capacity, flexible lithium‐ion battery is fabricated using a new nanofibril‐structured silicon anode on a flexible current collector. Silicon is known to be the highest capacity anode material. However, its huge volume changes during the lithium insertion and extraction results in pulverization, which is the cause of the rapid capacity fade that occurs as the charge‐discharge cycles progress. Nanostructured silicon can overcome this pulverization problem. A flexible current collector with high electric conductivity is prepared by a RF‐magnetron sputtering of a thin copper layer (<1 μm) onto a porous polymeric membrane. This provides not only flexibility of the electrode but also a template for simple fabrication of nanostructured silicon. Cells using the new, flexible current collector and corresponding silicon nanofibril‐structured anode exhibit energy capacities over 2000 mAh g^?1 during 30 charge‐discharge cycles at C/2. In addition, the coulombic efficiency remains over 99% after the third cycle. These results demonstrate the potential of the new anode for use in commercial high‐capacity, flexible lithium‐ion batteries.     

A Lithium‐Sulfur Battery with a High Areal Energy Density

The battery community has recently witnessed a considerable progress in the cycle lives of lithium‐sulfur (Li‐S) batteries, mostly by developing the electrode structures that mitigate fatal dissolution of lithium polysulfides. Nonetheless, most of the previous successful demonstrations have been based on limited areal capacities. For realistic battery applications, however, the chronic issues from both the anode (lithium dendrite growth) and the cathode (lithium polysulfide dissolution) need to be readdressed under much higher loading of sulfur active material. To this end, the current study integrates the following three approaches in a systematic manner: 1) the sulfur electrode material with diminished lithium polysulfide dissolution by the covalently bonded sulfur‐carbon microstructure, 2) mussel‐inspired polydopamine coating onto the separator that suppresses lithium dendrite growth by wet‐adhesion between the separator and Li metal, and 3) addition of cesium ions (Cs⁺) to the electrolyte to repel incoming Li ions and thus prevent Li dendrite growth. This combined strategy resolves the long‐standing problems from both electrodes even under the very large sulfur‐carbon composite loading of 17 mg cm^?2 in the sulfur electrode, enabling the highest areal capacity (9 mAh cm^?2) to date while preserving stable cycling performance.     

Layered Silicon‐Based Nanosheets as Electrode for 4 V High‐Performance Supercapacitor

Silicon‐based materials have shown great potential and been widely studied in various fields. Unlike its unparalleled theoretical capacity as anodes for batteries, few investigations have been reported on silicon‐based materials for applications in supercapacitors. Here, an electrode composed of layered silicon‐based nanosheets, obtained through oxidation and exfoliation, for a supercapacitor operated up to 4 V is reported. These silicon‐based nanosheets show an areal specific capacitance of 4.43 mF cm^?2 at 10 mV s^?1 while still retaining a specific capacitance of 834 µF cm^?2 even at an ultrahigh scan rate of 50 000 mV s^?1. The volumetric energy and power density of the supercapacitor are 7.65 mWh cm^?3 and 9312 mW cm^?3, respectively, and the electrode can operate for 12000 cycles in a potential window of 4 V at 2 A g^?1, while retaining 90.6% capacitance. These results indicate that the silicon‐based nanosheets can be a competitive candidate as the supercapacitor electrode material.     

Sputtered Titanium Carbide Thick Film for High Areal Energy on Chip Carbon‐Based Micro‐Supercapacitors

The areal energy density of on‐chip micro‐supercapacitors should be improved in order to obtain autonomous smart miniaturized sensors. To reach this goal, high surface capacitance electrode (>100 mF cm^?2) has to be produced while keeping low the footprint area. For carbide‐derived carbon (CDC) micro‐supercapacitors, the properties of the metal carbide precursor have to be fine‐tuned to fabricate thick electrodes. The ad‐atoms diffusion process and atomic peening effect occurring during the titanium carbide sputtering process are shown to be the key parameters to produce low stress, highly conductive, and thick TiC films. The sputtered TiC at 10^?3 mbar exhibits a high stress level, limiting the thickness of the TiC‐CDC electrode to 1.5 µm with an areal capacitance that is less than 55 mF cm^?2 in aqueous electrolyte. The pressure increase up to 10^?2 mbar induces a clear reduction of the stress level while the layer thickness increases without any degradation of the TiC electronic conductivity. The volumetric capacitance of the TiC‐CDC electrodes is equal to 350 F cm^?3 regardless of the level of pressure. High values of areal capacitance (>100 mF cm^?2) are achieved, whereas the TiC layer is relatively thick, which paves the way toward high‐performance micro‐supercapacitors.