The demineralization of dental hard tissue imposes considerable health and economic burdens worldwide, but an optimal method that can repair both the chemical composition and complex structures has not been developed. The continuous development of nanotechnology has created new opportunities for the regeneration and repair of dental hard tissue. Increasingly studies have reported that nanomaterials (NMs) can induce and regulate the biomimetic mineralization of dental hard tissue, but few studies have examined how they are involved in the different stages, let alone the relevant mechanisms of action. Besides their nanoscale dimensions and excellent designability, NMs play a corresponding role in the function of the raw materials for mineralization, mineralized microenvironment, mineralization guidance, and the function of mineralized products. This review comprehensively summarizes the advantages of NMs and examines the specific mineralization mechanisms. Design strategies to promote regeneration and repair are summarized according to the application purpose of NMs in the oral cavity, and limitations and development directions in dental hard tissue remineralization are proposed. This review can provide a theoretical basis to understand the interaction between NMs and the remineralization of dental hard tissue, thereby optimizing design strategy, rational development, and clinical application of NMs in the field of remineralization.