In the past few decades, various vanadium compounds have displayed potential in cancer treatment. However, fast clearness in the body and possible toxicity of vanadium compounds has hindered their further development. Vanadium-based nanomaterials not only overcome these limitations, but take advantage of the internal properties of vanadium in photics and magnetics, which enable them as a multimodal platform for cancer diagnosis and treatment. In this paper, we first introduced the basic biological and pharmacological functions of vanadium compounds in treating cancer. Then, the synthesis routes of three vanadium-based nanomaterials were discussed, including vanadium oxides, 2D vanadium sulfides, carbides and nitrides: VmXn (X = S, C, N) and water-insoluble vanadium salts. Finally, we highlighted the applications of these vanadium-based nanomaterials as tumor therapeutic and diagnostic agents.