Developing an integrated multimodal diagnosis and therapeutics nanoplatform is of great importance to enhance the outcome of cancer therapy. Herein, we report a highly efficient and biocompatible nanoplatform based on the assembly of a graphene oxide (GO) and metal–organic framework (MOF) Fe–porphyrin, which was coated with a folate-functionalized erythrocyte membrane (FA-EM@GO-MOF). The nanoplatform could be targeted to cancer cells precisely, and could avoid immune elimination and had prolonged blood circulation due to the presence of FA-EM on its surface. The presence of GO and paramagnetic Fe ions endowed the nanoplatform with robust fluorescence imaging and T₂-weighted magnetic resonance imaging capacities. The porous structure and large surface area of GO-MOF make it desirable for drug delivery in chemotherapy. More importantly, with one operation, under the same laser (808 nm) irradiation, both photothermal therapy and photodynamic therapy could be triggered for efficient synergistic treatment by using MOF as a photosensitizer. This synergistic anticancer therapy promoted the generation of tumor-associated antigens and evoked an antitumor immune response. In vitro and in vivo therapy studies highlighted that the as-fabricated biomimetic nanoplatform for dual imaging-guided synergistic cancer therapy was highly effective yet straightforward, paving a new avenue for cancer diagnosis and therapy.