VS₄‐Anchored Carbon Nanofiber Network with MXene Coating as Flexible and Self‐Supported Electrode for Rapid and Durable Lithium Storage

The high sulfur content and unique chain structure of VS 4 make it a promising electrode material, while its further application is limited by the unsatisfactory Li + diffusion kinetics, structural instability, and challenges in achieving flexible energy storage. Here, a VS 4 ‐anchored, N‐doped carbon nanofibers (N‐CNFs) network with MXene shell and surface coating is constructed, enabling durable and fast Li + storage in batteries. This flexible and self‐supported electrode demonstrates high reversible capacity (1350 mAh g −1 at 0.1 A g −1 ), excellent rate (430 mAh g −1 at 10 A g −1 ) and cycling (453 mAh g −1 after 2000 cycles at 5 A g −1 ) performance. The 3D N‐CNFs substrate, with large surface area, mechanical flexibility, and high conductivity, forms a robust interfacial bond with the anchored VS 4 , thereby enhancing structural stability. The optimized MXene‐VS 4 interfacial structure is revealed to enhance Li + adsorption, shorten Li + transport pathways, and effectively buffer the volume changes of VS 4 . When paired with NCM8 11 and LFP cathodes, the flexible pouch cells exhibit high capacities and robust cycling performance under bending conditions. This strategic layered design enhances the reaction kinetics and stability of VS 4 for Li + storage, offering a promising electrode design strategy for fast‐charging flexible batteries.