We report a facile strategy to fabricate well-dispersed Fe3O4@C eccentric core-shell nanoparticles (NPs). The resulting Fe3O4@C eccentric core-shell NPs possess a high payload of doxorubicin (DOX) for use as synergetic pH/near-infrared (NIR)-sensitive drug delivery vehicles, and were applied for dual-modal magnetic resonance imaging (MRI)/photoacoustic imaging (PAI) and synergistic photothermal cancer therapy in vitro and in vivo.