Shape editability combined with a self‐healing capability and long‐term cycling durability are highly desirable properties for wearable supercapacitors. Most wearable supercapacitors have rigid architecture and lack the capacity for editability into desirable shapes. Through sandwiching hydrogel electrolytes between two electrodes, a suite of wearable supercapacitors that integrate desirable properties namely: repeated shape editability, excellent self‐healing capability, and long‐term cycling durability is demonstrated. A strategy is proposed to enhance the long‐term cycling durability by utilizing hydrogel electrolytes with unique cross‐linking structures. The dynamic crosslinking sites are formed by quadruple H bonds and hydrophobic association, stabilizing the supercapacitors from inorganic ion disruption during charge–discharge processes. The fabricated supercapacitors result in the capacitance retention rates of 99.6% and 95.8% after 5000 and 10 000 charge–discharge cycles, respectively, which are much higher than others reported in the literature. Furthermore, the supercapacitor sheets can be repeatedly processed into various shapes without any capacitance loss. The supercapacitors exhibit a 95% capacitance retention rate after five cutting/self‐healing cycles, indicative of their excellent self‐healing performance. To demonstrate real‐life applicability, the wearable supercapacitors are successfully used to power a light‐emitting diode and an electronic watch.

Thermoformable bionanocomposites of chitin whisker-graft-polycaprolactone (CHW-g-PCL) were synthesized by initiating the ring-opening polymerization of caprolactone monomer onto the CHW surface under microwave radiation. In this case, the ''graft from'' strategy contributed to long and dense ''plasticizing'' PCL tails onto the CHW surface as the key of thermoforming, and, therefore, such bionanocomposites were injection-molded as the sheets with a structure of cocontinuous phase mediated with the entanglement of grafted PCL chains. The structure and properties of the molded CHW-g-PCL sheets were investigated by FTIR, XRD, SEM, DSC, DMTA, contact angle measurement, and tensile test. With an increase of the PCL content in CHW-g-PCL, the strength and elongation as well as the hydrophobicity of the nanocomposites increased at one time. This is the first report on the thermoformable polymer-grafted nanocrystal derived from natural polysaccharide. Moreover, such new bionanocomposites with good mechanical performances could have great potential applications.