Chemical architectures with an ordered porous backbone and high charge transfer are significant for fibershaped supercapacitors (FSCs). However,o wingt ot he sluggish ion kinetic diffusion and storage in compacted fibers, achieving high energy density remains ac hallenge.A n innovative magnetothermal microfluidic method is now proposed to design hierarchicalc arbon polyhedrons/holey graphene (CP/HG) core-shell microfibers.O wing to highly magnetothermal etching and microfluidic reactions,t he CP/ HG fibers maintain an open inner-linked ionic pathway,large specific surface area, and moderate nitrogen active site, facilitating more rapid ionic dynamic transportation and accommodation. The CP/HG FSCs showa nu ltrahigh energy density (335.8 mWh cm À2 )a nd large areal capacitance (2760 mF cm À2 ). As elf-powered endurance application with the integration of chip-based FSCs is designed to profoundly drive the durable motions of an electric car and walking robot.

Graphene oxide (GO) has aroused worldwide interests in recent years because of perfect solubility, easy processing nature, and intriguing mechanical properties. However, safety risk, high pollution, and low synthesis rate involved in the synthesis process of GO limit its practical applications. In this work, we propose a new strategy to efficiently produce the high-quality GO based on microfluidic synthesis technology. By use of the H2SO4/H3PO4/graphite hybrid microdroplet as the microreactor, the exfoliation and oxidation of graphite can be confined in a microscale reaction environment, indicating the enhanced reaction kinetics, high reaction rate (reaction time of 2 h), and minimum safety risk. Notably, the microfluidic synthesis of GO has nearly the same chemical structure when compared with the Hummers method. More importantly, the rGO fibers processed from GO solutions possess a high specific capacitance of 716.2 mF cm–2 (23.86 F g–1) and an energy density of 14.5 μWh cm–2 (0.53 Wh kg–1), which can enduringly power a smart watch. These versatile strategies open a promising access to the fast synthesis and commercial applications of graphene.

Chemical architectures with an ordered porous backbone and high charge transfer are significant for fiber‐shaped supercapacitors (FSCs). However, owing to the sluggish ion kinetic diffusion and storage in compacted fibers, achieving high energy density remains a challenge. An innovative magnetothermal microfluidic method is now proposed to design hierarchical carbon polyhedrons/holey graphene (CP/HG) core–shell microfibers. Owing to highly magnetothermal etching and microfluidic reactions, the CP/HG fibers maintain an open inner‐linked ionic pathway, large specific surface area, and moderate nitrogen active site, facilitating more rapid ionic dynamic transportation and accommodation. The CP/HG FSCs show an ultrahigh energy density (335.8 μWh cm−2) and large areal capacitance (2760 mF cm−2). A self‐powered endurance application with the integration of chip‐based FSCs is designed to profoundly drive the durable motions of an electric car and walking robot.

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Two‐dimensional transition metal titanium carbide (Ti3C2Tx) as a promising candidate material for batteries and supercapacitors has shown excellent electrochemical performance, but it is difficult to meet practical applications because of its poor morphology structure, low mechanical properties, and expensive process. Here, an applied and efficient method based on microfluidic wet‐fusing spinning chemistry (MWSC) is proposed to construct hierarchical structure of MXene‐based fiber fabrics (MFFs), allowing the availability of MFF electrodes with ultrastrong toughness, high conductivity, and easily machinable properties. First, a dot‐sheet structure constructed by graphene quantum dots (GQDs) and MXene nanosheets with multianchor interaction in the microchannel of a microfluidic device enhances the mechanical strength of MXene fibers; next, the interfused fiber network structure of Ti3C2Tx/GQDs fabrics assembled by the MWSC process enhances the deformability of the whole fabrics; finally, the core–shell structure of PANI@Ti3C2Tx/GQDs architected by in‐situ polymerization growth of polyaniline (PANI) nanofibers provides more ion‐accessible pathways and sites for kinetic migration and ion accumulation. Through the morphology and microstructure design, this strategy has directive significance to the large‐scale preparation of conductive fabric electrodes and provides a viable solution for simultaneously enhancing mechanical strength and electrochemical performance of conductive fabric electrodes.