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Photocatalytic H 2 O 2 evolution through two-electron oxygen reduction has attracted wide attention as an environmentally friendly strategy compared with the traditional anthraquinone or electrocatalytic method. Herein, a biomimetic leaf-vein-like g-C 3 N 4 as an efficient photocatalyst for H 2 O 2 evolution is reported, which owns tenable band structure, optimized charge transfer, and selective two-electron O 2 reduction. The mechanism for the regulation of band structure and charge transfer is well studied by combining experiments and theoretical calculations. The H 2 O 2 yield of CN4 (287 µmol h −1) is about 3.3 times higher than that of pristine CN (87 µmol h −1), and the apparent quantum yield for H 2 O 2 evolution over CN4 reaches 27.8% at 420 nm, which is much higher than that for many other current photocatalysts. This work not only provides a novel strategy for the design of photocatalyst with excellent H 2 O 2 evolution efficiency, but also promotes deep understanding for the role of defect and doping sites on photocatalytic activity.

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