Microstructure Design of Carbonaceous Fibers: A Promising Strategy toward High‐Performance Weaveable/Wearable Supercapacitors

Fiber‐based supercapacitors (FSCs) possess great potential as an ideal type of power source for future weaveable/wearable electronics and electronic‐textiles. The performance of FSCs is, without doubt, primarily determined by the properties of fibrous electrodes. Carbonaceous fibers, e.g., commercial carbon fibers, newly developed graphene fibers, and carbon nanotube fibers, are deemed as promising materials for weaveable/wearable supercapacitors owing to their exotic properties including high tensile strength and robustness, excellent electrical conductivity, good flexibility, and environmental stability. Nevertheless, bare carbonaceous fiber normally exhibits low capacitance originating from electric double‐layer capacitance, which remains unsatisfactory for efficiently powering wearable and portable devices. Numerous efforts have been devoted to tailoring fiber properties by hybridizing pseudocapacitive materials, and impressive progress has been achieved thus far. Herein, the microstructures of pristine carbonaceous fibers are introduced in detail, and the recent advances in rational nano/microstructure design of their hybrids, which provides the feasibility to achieve the synergistic interaction between conductive agents and pseudocapacitive nanomaterials but are normally overlooked, are comprehensively reviewed. Besides, the challenges in developing high‐performance fibrous electrodes are also elaborately discussed. Fiber‐based supercapacitors (FSCs) have attracted significant interests since they possess great potential as an ideal type of power sources for future wearable electronics and electronic textiles. This review systematically summarizes recently reported carbonaceous fibers and their hybrids for FSCs, focusing on the advances and challenges of their microstructure designs.