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Atomically thin two-dimensional (2D) CN sheets have attracted extensive attention in the field of photocatalysis because of their shorter diffusion path of photogenerated carriers and abundant surface reaction sites than bulk CN. However, 2D CNs still exhibit poor visible-light photocatalytic activity because of a strong quantum size effect. Here, PCN-222/CNs vdWHs were successfully constructed using the electrostatic self-assembly method. The results showed that PCN-222/CNs vdWHs with 1 wt.% PCN-222 enhanced the absorption range of CNs from 420 to 438 nm, which improved the absorption capacity of visible light. Additionally, the hydrogen production rate of 1 wt.% PCN-222/CNs is four times that of the pristine 2D CNs. This study provides a simple and effective strategy for 2D CN-based photocatalysts to promote visible light absorption.