Emerging autonomous electronic devices require increasingly compact energy generation and storage solutions. Merging these two functionalities in a single device would significantly increase their volumetric performance, however this is challenging due to material and manufacturing incompatibilities between energy harvesting and storage materials. Here we demonstrate that organic-inorganic hybrid perovskites can both generate and store energy in a rechargeable device termed a photobattery. This photobattery relies on highly photoactive two-dimensional lead halide perovskites to simultaneously achieve photocharging and Li-ion storage. Integrating these functionalities provides simple autonomous power solutions while retaining capacities of up to 100 mAh/g and efficiencies similar to electrodes using a mixture of batteries and solar materials. © 2018 American Chemical Society.