The booming wearable/portable electronic devices industry has stimulated the progress of supporting flexible energy storage devices. Excellent performance of flexible devices not only requires the component units of each device to maintain the original performance under external forces, but also demands the overall device to be flexible in response to external fields. However, flexible energy storage devices inevitably occur mechanical damages (extrusion, impact, vibration)/electrical damages (overcharge, over-discharge, external short circuit) during long-term complex deformation conditions, causing serious performance degradation and safety risks. Inspired by the healing phenomenon of nature, endowing energy storage devices with self-healing capability has become a promising strategy to effectively improve the durability and functionality of devices. Herein, this review systematically summarizes the latest progress in intrinsic self-healing chemistry for energy storage devices. Firstly, the main intrinsic self-healing mechanism is introduced. Then, the research situation of electrodes, electrolytes, artificial interface layers and integrated devices based on intrinsic self-healing and advanced characterization technology is reviewed. Finally, the current challenges and perspective are provided. We believe this critical review will contribute to the development of intrinsic self-healing chemistry in the flexible energy storage field.