The emergence of flexible and wearable electronic devices with shape amenability and high mobility has stimulated the development of flexible power sources to bring revolutionary changes to daily lives. The conventional rechargeable batteries with fixed geometries and sizes have limited their functionalities in wearable applications. The first‐ever graphene‐based fibrous rechargeable batteries are reported in this work. Ultralight composite fibers consisting of reduced graphene oxide/carbon nanotube filled with a large amount of sulfur (rGO/CNT/S) are prepared by a facile, one‐pot wet‐spinning method. The liquid crystalline behavior of high concentration GO sheets facilitates the alignment of rGO/CNT/S composites, enabling rational assembly into flexible and conductive fibers as lithium–sulfur battery electrodes. The ultralight fiber electrodes with scalable linear densities ranging from 0.028 to 0.13 mg cm−1 deliver a high initial capacity of 1255 mAh g−1 and an areal capacity of 2.49 mAh cm−2 at C/20. A shape‐conformable cable battery prototype demonstrates a stable discharge characteristic after 30 bending cycles.

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SnS2 nanoplatelet electrodes can offer an exceptionally high pseudocapacitance in an organic Na+ ion electrolyte system, but their underlying mechanisms are still largely unexplored, hindering the practical applications of pseudocapacitive SnS2 anodes in Na‐ion batteries (SIBs) and Na hybrid capacitors (SHCs). Herein, SnS2 nanoplatelets are grown directly on SnO2/C composites to synthesize SnS2/graphene‐carbon nanotube aerogel (SnS2/GCA) by pressurized sulfidation where the original morphology of carbon framework is preserved. The composite electrode possessing a large surface area delivers a remarkable specific capacity of 600.3 mA h g−1 at 0.2 A g−1 and 304.8 mA h g−1 at an ultrahigh current density of 10 A g−1 in SIBs. SHCs comprising a SnS2/GCA composite anode and an activated carbon cathode present exceptional energy densities of 108.3 and 26.9 W h kg−1 at power densities of 130 and 6053 W kg−1, respectively. The in situ transmission electron microscopy and the density functional theory calculations reveal that the excellent pseudocapacitance originates from the combination of Na adsorption on the surface/Sn edge of SnS2 nanoplatelets and ultrafast Na+ ion intercalation into the SnS2 layers.