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Multifunctional theranostic agents are widely applied in cancer diagnosis and treatment. These agents can significantly improve therapeutic outcomes and reduce adverse effects in current cancer therapy. Here, we have designed and synthesized iron-doped copper sulfide nanoparticles with polyvinylpyrollidone (FCS@PVP NPs) for magnetic resonance imaging (MRI) guided photothermal therapy. The biocompatible FCS@PVP NPs with strong near-infrared absorption could be used as the photothermal agent and the magnetic characteristic of Fe3+ ions could be applied to T1-weighted magnetic resonance imaging (MRI). The T1-weighted MRI, high photothermal performance, and the biodistribution of FCS@PVP NPs were investigated in mice after intravenous administration. The data showed that there was a high accumulation of FCS@PVP NPs in the tumor sites because of the enhanced permeability and retention (EPR) effect. This result also indicated that the tumors in tumor-bearing mice were effectively suppressed after FCS@PVP NPs treatment under 808 nm laser irradiation. More importantly, FCS@PVP NPs show low cytotoxicity and few side effects because of the quick and safe elimination through the hepatobiliary/fecal route. This work provided a foundation for the clinical application of FCS@PVP NPs as a promising multifunctional theranostic agent for the MRI guided photothermal therapy of cancer. [ABSTRACT FROM AUTHOR]