Coordination Polyphenol and Hydrogenation Coarmed Ce−Mo Bimetal Nanozymes for Robust Anticancer Therapy

Abstract Molybdenum oxide (MoO x ), which exhibits localized surface plasmon resonance and intrinsic enzyme‐mimicking activity, holds great promise as a photoresponsive nanozyme in cancer therapy. However, its narrow light absorption range and poor charge separation hinder its catalytic performance. Here, cerium (Ce) doping and hydrogenation narrow the bandgap of MoO x from 3.02 to 1.14 eV, enabling efficient photocarrier separation under 1064 nm irradiation and promoting O 2 to 1 O 2 conversion. Ce doping introduces Mo−O−Ce bridges, facilitating charge transfer via d–f orbital hybridization and modulating the d‐band center, which optimizes intermediate desorption at Mo sites and enhances the peroxidase‐like activity for •OH generation. Simultaneously, the intrinsic catalase‐like function generates O 2 , that supplies the substrate for photodynamic therapy (PDT). The hydrogenated MoO x is coated with a metal polyphenol network composed of Ce and epigallocatechin gallate, enabling it to reach the tumor sites safely. The final nanozyme system obtains under 1064 nm irradiation (denoted as HCMM@E‐Ce) achieves synergistic photothermal therapy, PDT, and enzymatic therapy, resulting in effective tumor suppression. This Ce 3+ ‐coordinated polyphenol and hydrogenation coarmed nanozyme platform integrates electronic structure modulation and tumor‐specific delivery, offering a promising strategy for precise and efficient cancer therapy.