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Modulating the electronic structure of cocatalysts is critical for designing active sites toward efficient photocatalytic H 2 evolution. Here, we report an electronic modulation in atomically dispersed Pt as highly efficient H 2 -evolution sites on graphitic carbon nitride (g-C 3 N 4 ) nanosheets. Synchrotron radiation X-ray spectroscopic results confirm the singly dispersed Pt atoms anchored on g-C 3 N 4 via forming "Pt 1 −N 4 " moiety, where the strong interaction of Pt with supports leads to the redistribution of Pt valence electrons with the highly vacant 5d orbital. Mechanistic investigations reveal that the immobilization of Pt single atoms with electron-deficient 5d orbitals on g-C 3 N 4 nanosheets not only facilitate the separation of electron−holes pair but also optimize the water reduction kinetics on the surface. As a result, the Pt single atoms photocatalyst achieves a high intrinsic activity with turnover frequency of 250 h −1 , about 13 times higher than the 19.5 h −1 of its nanocrystal counterpart.

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