Though there already had been notable progress in developing efficient therapeutic strategies for cancers, there still exist many requirements for significant improvement of the safety and efficiency of targeting cancer treatment. Thus, the rational design of a fully biodegradable and synergistic bioimaging and therapy system is of great significance. Metal organic framework (MOF) is an emerging class of coordination materials formed from metal ion/ion clusters nodes and organic ligand linkers. It arouses increasing interest in various areas in recent years. The unique features of adjustable composition, porous and directional structure, high specific surface areas, biocompatibility, and biodegradability make it possible for MOFs to be utilized as nano-drugs or/and nanocarriers for multimodal imaging and therapy. This review outlines recent advances in developing MOFs for multimodal treatment of cancer and discusses the prospects and challenges ahead.