With the development of enzymes immobilization technology and the discover of nanozymes, catalytic therapy exhibited tremendous potential for neurological diseases therapy. In especial, since the discovery of Fe₃O₄ nanoparticles possessing intrinsic peroxidase-like activity, various nanozymes have been developed and recently started to explore for neurological diseases therapy, such as Alzheimer's disease, Parkinson's disease and stroke. By combining the catalytic activities with other properties (such as optical, thermal, electrical, and magnetic properties) of nanomaterials, the multifunctional nanozymes would not only alleviate oxidative and nitrosative stress on the basis of multienzymes-mimicking activity, but also exert positive effects on immunization, inflammation, autophagy, protein aggregation, which provides the foundation for multifaceted treatments. This review will summarize various types of nanocatalysts and further provides a valuable discussion on multifaceted treatment by nanozymes for neurological diseases, which is anticipated to provide an easily accessible guide to the key opportunities and current challenges of the nanozymes-mediated treatments for neurological diseases.