Multiple Heteroatom‐Hydrogen Bonds Bridging Electron Transport in Covalent Organic Framework‐Based Supramolecular System for Photoreduction of CO2

-to-CO conversion, far superior to photosystems with supported atomic Ni or metal complex alone in the absence of hydrogen-bond effect. Such heteroatom-hydrogen bonds bridging electron transport pathway confers supramolecular system with high photocatalytic performance, providing an avenue to rationally design efficient and steadily available photosystems.