Metals are essential components in living systems. Metal ions as well as metalloproteins play an important role in almost all life processes, including materials storage and transportation, energy conversion and transfer, signal transduction and regulation, and molecules synthesis and degradation. Metals are also key players in immune system, especially the regulation of immune response, and misregulation of metals often cause a broad range of diseases. In recent years, cancer immunotherapy has shown significant promise and made people see the hope of curing cancer. The important role of metal elements in immune response and cancer therapy is gradually receiving attention and is the future direction in cancer immune; however, most of current research only have phonotypical descriptions but limited to clear molecular mechanism. This paper will briefly introduce the pivotal role of metal elements in the immune response process as well as their cutting-edge applications in cancer immunotherapy, and clarify the research category, scientific value and future development of this emerging frontier, which we terms as “Metalloimmunology”.