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Carbon is ubiquitously used as catalyst supports in various clean energy technologies, particularly emerging electrocatalysis, yet it often suffers slow oxidation and corrosion along with performance degradation. The harmonious combination of refractory silicon carbide (SiC, chemically inert) with carbon is alluring but often a great challenge, particularly to achieve desirable nanostructures and strong interfaces. Herein, a shockwave‐type transient heating is designed (> 1750 °C for 1 s per pulse) for controllable growth of conformal SiC coating and massive SiC nanowires on carbon fibers (denoted as CF/SiC‐NW), which serves as a high surface area and durable support for catalysis under harsh environments. The transient heating in SiO vapor triggers in situ transformation of the carbon surface into a seamless SiC protective layer, while the following fast cooling is essential for the growth of numerous self‐assembled SiC nanowires. The CF/SiC‐NW exhibits excellent structural stability in the air at high temperatures, in concentrated acidic/alkaline solutions after electrochemical stressing for 2000 cycles, and in oxygen evolution reaction after 10 h of continuous operation. This strategy enables delicate structure control in refractory carbides and is also general for various carbon/carbide functional materials (e.g., C/TiC, C/WC) for electro‐ or electrified catalysis under harsh conditions.

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Layered double hydroxide (LDH) is widely used in electrocatalytic water splitting due to its good structural tunability, high intrinsic activity, and mild synthesis conditions, especially for flexible fiber-based catalysts. However, the poor stability of the interface between LDH and flexible carbon textile prepared by hydrothermal and electrodeposition methods greatly affects its active area and cyclic stability during deformation. Here, we report a salt-template-assisted method for the growth of two-dimensional (2D) amorphous ternary LDH based on dip-rolling technology. The robust and high-dimensional structure constructed by salt-template and fiber could achieve a carbon textile-based water splitting catalyst with high loading, strong catalytic activity, and good stability. The prepared 2D NiFeCo-LDH/CF electrode showed overpotentials of 220 mV and 151 mV in oxygen evolution and hydrogen evolution reactions, respectively, and simultaneously had no significant performance decrease after 100 consecutive bendings. This work provides a new strategy for efficiently designing robust, high-performance LDH on flexible fibers, which may have great potential in commercial applications.

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