Exploiting new non-metal-based peroxidase-mimic nanoenzymes for chemodynamic therapy (CDT) in cancer treatment is an active and challenging field. Here, we found that activated carbon nanoparticles (denoted as ANs) fabricated from coconut shell have satisfactory peroxidase-mimic nanoenzyme activity. Based on this positive result, gadodiamide, a clinically used nuclear magnetic imaging contrast agent, was loaded inside the AN pores and encapsulated by polyvinylpyrrolidone (PVP) to obtain Gd@PANs. PANs (ANs modified using PVP) efficiently catalyze the massive decomposition of endogenous hydrogen peroxide (H2O2) inside cancer cells to produce toxic oxidized hydroxyl radicals (˙OH) for the CDT treatment of cancer, but they showed no toxicity toward normal cells. Additionally, under 808 nm laser irradiation, the photothermal conversion efficiency of the PANs reaches 45.20%, ensuring their effective photothermal therapy (PTT) treatment functionality. Simultaneously, during PTT treatment, the heating effect significantly enhances the peroxidase-mimic activity of the PANs to achieve an ideal PTT-CDT synergistic therapeutic outcome. Gd@PANs can also be used for the T1-magnetic resonance imaging (MRI) of tumors to integrate treatment and diagnosis.