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Near‐infrared (NIR) light‐driven overall water splitting beyond 800 nm remains a high‐priority target yet great challenge. Here we report that efficient utilization of photogenerated electrons in a photosensitized system prepared by site‐selective photodeposition of platinum single atoms/clusters (Pt‐SACs) on Ni‐phytate (PA‐Ni)‐sensitized polymeric carbon nitride (PCN). The optimal catalyst presents simultaneous hydrogen (H2) and oxygen (O2) evolution with an H2 evolution amount of 1.4 μmol at λ>800 nm for 24 hours, which its activity was approximately 140 times higher than that of a system without Pt‐SAC modification (PA‐Ni1.1@PCN). This work represents the first NIR‐light responsive photosensitized system for overall water splitting, and may open an avenue for precisely manipulating cocatalyst positions at the atomic level to improve NIR‐light‐driven overall water splitting via photosensitization. [ABSTRACT FROM AUTHOR]