Malignant primary brain tumors have a very high morbidity and mortality. Even though enormous advances have been made in primary brain tumor management, in the case of malignant primary brain tumors, current diagnostic strategies cannot identify exact in¯ltrating margins, surgery alone cannot achieve total mass resection, and adjuvant therapies cannot improve survivals. Therefore, there is an urgent need to explore novel strategies to diagnose and treat such in¯ltrating brain tumors. Nanomaterials, particularly zero-dimensional and one-dimensional platforms, can carry various compounds such as contrast agents, anticancer drugs and genes into brain tumor cells speci¯cally. Thus, contrast agent-based nanomaterials can selectively present in¯ltrating tumor outlines, while anticancer agent-based nanomaterials can speci¯cally kill malignant tumor cells. In addition, dual-targeting nanomaterials, multifunctional nanocarriers, theranostic nanovehicles as well as convection-enhanced delivery technology hold promise to increase drug accumulation in tumor tissues, which could largely improve anticancer e±cacy. In this review, we will mainly focus on the application of nanomaterials in preoperative diagnosis, intraoperative diagnosis and adjuvant treatment for malignant primary brain tumors.