Metal–organic frameworks (MOFs) are a class of multifunctional organometallic compounds that include metal ions combined with assorted organic linkers. Recently, these compounds have received widespread attention in medicine, due to their exceptional qualities, including a wide surface area, high porosity, outstanding biocompatibility, non-toxicity, etc. Such characteristic qualities make MOFs superb candidates for biosensing, molecular imaging, drug delivery, and enhanced cancer therapies. This review illustrates the key attributes of MOFs and their importance in cancer research. The structural and synthetic aspects of MOFs are briefly discussed with primary emphasis on diagnostic and therapeutic features, as well as their performance and significance in modern therapeutic methods and synergistic theranostic strategies including biocompatibility. This review offers cumulative scrutiny of the widespread appeal of MOFs in modern-day oncological research, which may stimulate further explorations.