| Summary: | Although graphitic carbon nitride nanosheets (CNs) with atomic thickness are considered as promising materials for hydrogen production, the wide band gap (3.06 eV) and rapid recombination of the photogenerated electron–hole pairs impede their applications. To address the above challenges, we synergized atomically thin CNs and graphene quantum dots (GQDs), which were fabricated as 2D/0D Van der Waals heterojunctions, for H<sub>2</sub> generation in this study. The experimental characterizations indicated that the addition of GQDs to the π-conjugated system of CNs can expand the visible light absorption band. Additionally, the surface photovoltage spectroscopy (SPV) confirmed that introducing GQDs into CNs can facilitate the transport of photoinduced carriers in the melon chain, thus suppressing the recombination of charge carriers in body. As a result, the H<sub>2</sub> production activity of the Van der Waals heterojunctions was 9.62 times higher than CNs. This study provides an effective strategy for designing metal-free Van der Waals hetero-structured photocatalysts with high photocatalytic activity.
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