Nanostructured metal-organic frameworks (N-MOFs) are crystalline coordination nanopolymers in which metals are conjugated with organic and inorganic linker molecules. At present, N-MOFs have attracted significant interest owing to their intrinsically high porosity and ultrahigh surface areas, which allow them to be loaded with a broad array of materials, including drug molecules. In addition, N-MOFs possess other unique properties, such as good mobility, high reactivity, outstanding stability, real-time intracellular pH sensitivity, photosensitization, and penetration ability, which make them suitable candidates as drug delivery carriers for cancer and other targeted therapies. The opportunity for using a diverse array of chemical building components in N-MOFs facilitates the formation of structures with preferred properties for targeted therapy. In this review, we focus on the synthesis, characterization and other potential applications of N-MOFs in targeted theranostic nanodrug for cancer therapy.