Nanozymes are a class of nanomaterials with enzyme-like catalytic activities. Due to their multiple catalytic activities, as well as their good stability, modifiable activity and other advantages over natural enzymes, they have a wide range of application prospects in sterilization, the treatment of inflammation, cancer, and neurological diseases, and other fields. In recent years, it has been found that various nanozymes have antioxidant activity, allowing them to simulate the endogenous antioxidant system and play an important role in cell protection. Therefore, nanozymes can be applied in the treatment of reactive oxygen species (ROS)-related neurological diseases. Another advantage of nanozymes is that they can be customized and modified in a variety of ways to increase their catalytic activity beyond that of classical enzymes. In addition, some nanozymes have unique properties, such as the ability to effectively penetrate the blood‒brain barrier (BBB) or to depolymerize or otherwise eliminate misfolded proteins, making them potentially useful therapeutic tools for the treatment of neurological diseases. Here, we review the catalytic mechanisms of antioxidant-like nanozymes, as well as the latest research progress and strategies for designing therapeutic nanozymes, aiming to promote the development of more effective nanozymes for the treatment of neurological diseases in the future.