This paper describes the development of mitoxantrone-loaded PEGylated graphene oxide/magnetite nanoparticles (PEG-GO/Fe3O4-MTX), and investigation of its preliminary drug delivery performance. For this, the GO was synthesized through oxidizing graphite powder, and subsequently carboxylated using a substitution nucleophilic reaction. The carboxylated GO (GO-COOH) was then conjugated with amine end-caped PEG chains by Steglich esterification. Afterward, GO-PEG/Fe3O4 nanocomposite was synthesized through the anchoring of Fe3O4 nanoparticles onto the surface of GO-PEG during the sonication. The biocompatibility and MTX-loading capacity of the synthesized GO-PEG/Fe3O4 nanocomposite were evaluated. The pH dependent drug release behavior and cytotoxicity effect of the MTX-loaded GO-PEG/Fe3O4 nanocomposite were also studied. According to biocompatibility, pH dependent drug release behavior as well as superior physicochemical and biological characteristics of graphene and magnetite nanoparticles, it is expected that the GO-PEG/Fe3O4 nanocomposite may be applied as de novo drug delivery system (DDS) for cancer therapy using both chemo- and photothermal therapy approaches.