Metal-organic frameworks (MOFs) are a novel class of porous materials made from metal ions and organic ligands, and have been widely explored as multifunctional nanoplatforms. MOFs present unique physicochemical characteristics, such as large surface area, tunable size and structure, and easy modification, thereby making them promising candidates for drug delivery, biomedical imaging, and therapeutic applications. Simultaneous utilization of organic linkers and various metal ions as the coordination centers provides possibility to generate multifunctional MOFs with a number of advantages. This feature article summarizes the development and modification of MOFs with emphasis on the recent progress of chemotherapy-based synergistic combination therapy and bioimaging techinques, including computed tomography (CT), magnetic resonance imaging (MRI), positron emission tomography (PET) and optical imaging (OI). Future prospects and challenges of MOFs in the research of translational medicine are also discussed.