AbstractTheragnostics represent a combination of therapy and diagnosis within one system. Herein, Fe3O4‐ZIF‐8 core–shell nanoparticles are developed and suggested as candidates for theragnostic applications in cancer treatment. A drug loaded metal–organic framework ZIF‐8 (zeolitic imidazolate framework‐8) represents the therapeutic tool, while the Fe3O4 core is included to enable the material visualization by magnetic resonance imaging (MRI). A reliable synthesis of Fe3O4‐ZIF‐8 core–shell nanoparticles of an average size below 100 nm is reported. The nanoparticles are characterized by FT‐IR, TGA, XRPD, TEM, STEM‐EDS, DLS, ICP‐OES, CHN‐elemental analysis, SQUID measurements, and MRI. Moreover, their chemical stability and in vitro cytotoxicity against fibroblast and selected cancer cell lines are evaluated. As a model drug, arsenic trioxide—a promising anticancer drug—is used. The drug release can be triggered by a pH change from 7.4 to 6.0 and the nanoparticles can be visualized by MRI in vitro, thus a potential theragnostic agent for cancer treatment is developed.