LAUSR

Flexible fibrous supercapacitors (FFS) are considered the next‐generation wearable energy storage devices because they provide reliable safety, eco‐friendliness, and high power density. In particular, the FFS is desirable for application to wearable electronics because it can overcome disadvantages of the lithium‐ion battery (LIB), such as the hazard of explosion and the complex manufacturing process. Nevertheless, the practical application of the FFS continues to be inhibited by the poor energy storage performance due to the limited specific surface area, poor electrical properties, and low wettability of the carbon fiber electrode. Herein, for the first time, the surface engineering of an FFS using nitrogen and fluorine codoped mesoporous carbon fibers (FFS‐NFMCF) is described, and the synergistic effect of porosity tuning and heteroatom codoping upon the electrochemical performance is demonstrated. The resultant supercapacitor shows a high specific capacitance of 243.9 mF cm−2 at a current density of 10.0 µA cm−2 and good ultrafast cycling stability with capacitance retention of 91.3% for up to 10 000 cycles at a current density of 250.0 µA cm−2. More interestingly, the FFS‐NFMCF exhibits good mechanical properties and remarkable safety in practical application, thus demonstrating its feasibility for use in wearable electronic textiles.