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We report nanoceria (NCeO2) decorated flower-like MoS2 nanoflakes as a nanozyme for cancer photothermal therapy (PTT). They exhibited enzyme-like activity for selectively killing tumor cells by ROS induction. The NCeO2 decoration significantly improved the photoconversion efficiencies (PCEs) of MoS2 nanoflakes when a NCeO2 concentration of ≤0.5 mg mL−1 was used for synthesis. The novel material demonstrated here showed high photostability and PCE, without any systemic toxicity for cancer PTT.