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The photo‐rechargeable supercapacitor enables the self‐powering of flexible wearable electronics. However, flexible wearable electronics require supercapacitors not only with excellent flexibility but also with high energy density. P‐diaminoazobenzene (P‐Azo) as a new type of organic electrode material with NN is directly connected to the benzene ring and forms a large π‐conjugated system, which makes it have a lower lowest unoccupied molecular orbital (LUMO) energy level, is beneficial to transfer of electrons, and increases the conductivity of organic molecules. In addition, NN can realize the transfer of two electrons, which makes P‐Azo have a higher energy density. Asymmetric flexible supercapacitors are fabricated by assembling P‐Azo, activated carbon, and an adhesive electrolyte, with 425.2 mW h cm−2 (55.19 Wh kg−1) energy density at a power density of 80 mW cm−2 (10.38 W kg−1), and 90.7% capacitance retention after 80 000 cycles of bending. In this work, supercapacitors and perovskite submodules are coupled to prepare a photo‐rechargeable supercapacitor to achieve a 7% overall energy‐conversion efficiency. Therefore, this supercapacitor paves a practical route for powering future wearable electronics.