Hydrogen gas is produced photocatalytically using 470 nm light, PVP-coated carbon quantum dots (CQDs) as the photosensitizer, and nickel nanoparticles (NiNPs) as the catalyst. The effect of the amount of polyvinylpyrrolidone (PVP) on the ability of the CQD/NiNP composites to catalyze proton reduction was studied. A maximum of 330 mmols H2/g CQD is produced using 68 μg ml−1 of CQDs and 6 μg ml−1 of NiNPs, with activity persisting for 4 h when 20 wt%- PVP-coated CQDs were used. The H2 production quantum yield under these conditions is 6%. It was found that composites having higher weight percent PVP had decreased rates of H2 production, but increased duration. Increasing the weight percent of PVP coating also increases the fluorescence quantum yield of CQDs. Fluorescence quenching titrations reveal that H2 production could occur by either a reductive or oxidative quenching mechanism. The nanomaterials, prepared using simple methods, are used as the photosensitizer and catalyst in the proton reduction system that operates using visible light.