HighlightsA hybrid co-catalysts system comprising Au nanoparticles (NPs) and PtSAs with different functions was constructed on the polymeric carbon nitride (PCN) surface by double-solvent method.For the dual co-catalysts, the Au NPs absorb relatively long-wavelength light to produce plasmonic hot-electrons, and the adjacent Pt single atoms (PtSAs) can trap the plasmonic hot-electrons effectively for H2evolution.The PtSAs–Au2.5/PCN exhibits excellent broad-spectrum photocatalytic H2evolution activity with the H2evolution rate of 8.8 mmol g−1h−1at 420 nm and 264 μmol g−1h−1at 550 nm, respectively.Supplementary InformationThe online version contains supplementary material available at 10.1007/s40820-023-01098-2.