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Therefore, the development of novel functional materials capable of effectively remodeling the TME and alleviating immunosuppression and therapeutic tolerance has become an important research direction in cancer therapy. In recent years, nanozymes, as a class of nanomaterials with enzyme-mimicking catalytic activity, have shown broad potential in TME intervention and the enhancement of cancer therapy owing to their excellent physicochemical stability, tunable structural properties, and multiple biomimetic enzyme-like activities. This review systematically summarizes recent advances in nanozyme-mediated regulation of the TME. First, the basic concepts, catalytic properties, and functional classifications of nanozymes are introduced. Subsequently, the mechanisms by which nanozymes remodel the TME and enhance cancer therapy are discussed from the key dimensions of the redox microenvironment, metabolic microenvironment, and immune microenvironment. 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