Vaccines, one of the most effective and powerful public health measures, have saved countless lives over the past century and still have a tremendous global impact. As an indispensable component of modern vaccines, adjuvants play a critical role in strengthening and/or shaping a specific immune response against infectious diseases as well as malignancies. The application of nanotechnology provides the possibility of precisely tailoring the building blocks of nanoadjuvants towards modern vaccines with the desired immune response. The last decade has witnessed great academic progress in inorganic nanomaterials for vaccine adjuvants in terms of nanometer-scale synthesis, structure control, and functionalization design. Inorganic adjuvants generally facilitate the delivery of antigens, allowing them to be released in a sustained manner, enhance immunogenicity, deliver antigens efficiently to specific targets, and induce a specific immune response. In particular, the recent discovery of the intrinsic immunomodulatory function of inorganic nanomaterials further allows us to shape the immune response towards the desired type and increase the efficacy of vaccines. In this article, we comprehensively review state-of-the-art research on the use of inorganic nanomaterials as vaccine adjuvants. Attention is focused on the physicochemical properties of versatile inorganic nanoadjuvants, such as composition, size, morphology, shape, hydrophobicity, and surface charge, to effectively stimulate cellular immunity, considering that the clinically used alum adjuvants can only induce strong humoral immunity. In addition, the efforts made to date to expand the application of inorganic nanoadjuvants in cancer vaccines are summarized. Finally, we discuss the future prospects and our outlook on tailoring inorganic nanoadjuvants towards next-generation vaccines.