Jiamin Liu, Yingxinjie Wang, Guohao Li, Aidi Fu, Jiale Fan, Shurui Cong, Lei Wang, Senlin Zhang, Xiuqiang Xie, Nan Zhang
ABSTRACT Photo‐rechargeable batteries, capable of simultaneous solar energy harvesting and storage, attract significant research interest as next‐generation autonomous power systems. The development of high‐efficiency photoactive electrodes is highly desirable for achieving practical performance. Herein, we report V 2 O 5 /CdS composites for photo‐rechargeable zinc‐ion batteries, which enable efficient light‐to‐electricity‐to‐chemical energy conversion through effective separation of photogenerated electron–hole pairs. The photocell can be charged by light without an external power supply, achieving a light conversion efficiency of 0.99%. Notably, under a high current density (4.0 A g −1 ), the capacity increases 24.1% to 301 mA h g −1 after illumination compared to that in dark conditions. This work provides fundamental insights into the mechanisms enabling high‐rate performance in photo‐rechargeable zinc‐ion batteries.