Abstract Grain boundary cracks in flexible perovskite films can be repaired by filling with self‐repairing polymers during the preparation and wearable operation. However, the self‐repairing polymers are commonly active through external heating or humidification treatments, which cannot match with the human body's temperature tolerance of wearable devices. Herein, a body temperature‐responsive shape memory polyurethane (SMPU) is demonstrated to achieve the real‐time mechanical self‐repairing of grain boundary cracks (~37°C). Furthermore, the strong intermolecular interaction between SMPU and the uncoordinated Pb2+ and I−, can reduce the trap density in perovskite films. The blade‐coated device achieves a power conversion efficiency (PCE) of 21.33%, which is among the best reported flexible perovskite solar cells (PSCs; 0.10 cm2). Importantly, the device with SMPU can recover more than 80% of the PCE after 6000 cycles (bending radius: 8 mm). Finally, the flexible PSCs are used for wearable solar power supply of a smartphone, which show great potential for self‐repairing wearable electronics.
