Superparamagnetic Fe3O4 supraparticles@MIL-100(Fe) core-shell nanostructure microspheres were successfully constructed by a facile step-by-step method. The polyacrylate formed in situ during the process of the preparation of Fe3O4 supraparticles not only acted as a stabilizer on the Fe3O4 nanoparticles surface, but also played a crucial role as a "bridge" in the initial stage of the framework components selectively assembly on the Fe3O4 supraparticle surfaces. The structure and composition of the obtained microspheres were characterized by SEM, TEM, DLS, XRD, FTIR, and TG analysis. The MPMS results revealed that the introduction of the MOF shells can inhibit the interplay among the neighboring Fe3O4 supraparticles while an external magnetic field applied. The well-dispersed microspheres are bio-compatible, which endow the microspheres great potential in drug targeting applications with enhanced efficiency. (C) 2015 Elsevier Inc. All rights reserved.