In the past decade, metal-organic frameworks (MOFs) have been extensively researched for biomedical applications, particularly drug storage, after proving to be excellent substitutes for traditional porous materials. Biomedical applications of MOFs have been greatly expedited with the recent integration of data science and molecular modelling approaches to experimental research, establishing them as essential elements in medical imaging, diagnostics, and regenerative medicine. In this review, to demonstrate the potential of MOFs in cutting-edge treatments for neurological and cancer diseases, we examined the molecular interactions between MOFs and biological systems and discussed the field’s opportunities and challenges.