Chiral nanomaterials are widely investigated over recent decades due to their biocompatibility and unique chiral effects. These key properties have significantly promoted the rapid development of chiral nanomaterials in bioengineering and medicine. In this review, the basic principles of constructing chiral nanomaterials along with the latest progress in research are comprehensively summarized. Then, the application of chiral nanomaterials for the diagnosis of neurodegenerative diseases (NDDs) is systematically described. In addition, the significant potential and broad prospects of chiral nanomaterials in the treatment of NDDs are highlighted from several aspects, including the disaggregation of neurofibrils, the scavenging of reactive oxygen species, regulation of the microbial-gut-brain axis, the elimination of senescent cells, and the promotion of directed differentiation in neural stem cells. Finally, a perspective of the challenges and future development of chiral nanomaterials for the treatment of NDDs is provided.