Recently, neurological disorders have led to a growing global burden of fatalities and disabilities. The limited capacity for natural self‐regeneration poses a significant challenge in repairing nervous system injuries, which is closely related to the complex microenvironment and nonregenerative nature of neurons. Metal–organic frameworks (MOFs), with their distinctive structure and properties including high surface area, porosity, tunability, stimuli‐responsive behavior, biocompatibility, and biodegradability, stand as an auspicious platform for devising therapeutic strategies aiming at nerve regeneration and repair. By taking advantage of these characteristics, researchers have the opportunity to explore innovative methods including endogenous stimulation, magnetic response therapy, phototherapy, ultrasound therapy, and drug delivery systems for the treatment of neurological diseases. Moreover, MOFs‐based stem cell therapy also is developed to inhibit neuroinflammation and oxidative stress, promote axon growth, regulate stem cell differentiation, promote nerve regeneration, and finally restore the function of injured nerves. In this paper, the preparation strategy and biological characteristics of MOFs, highlighting their applications in repairing nerve injuries and treating neural stem cells is presented. Finally, an outlook on the future development and challenges in the field of neuroscience concerning MOFs is provided.