Self-healing single crystals, which possess the ability to recover from damage, represent an emerging filed within dynamic single-crystal materials. These materials not only deepen our understanding of the flexible structures inherent in single crystals but also offer a novel pathway for the development of smart materials, including soft robots, microelectronic devices, and optical devices. In this perspective, we provide a comprehensive summary of recent advancements in organic self-healing single crystals, highlighting various self-healing mechanisms, typical molecular structures, and the testing methods utilized to investigate these materials. We hope that our systematic overview of this field will significantly contribute to the advancement of self-healing single crystal materials as a new class of molecular-based functional materials, particularly in the integration of self-healing properties with innovative optoelectronic functionalities.