Abstract We report on the capability of polydopamine (PDA), a mimic of mussel adhesion proteins, as an electron gate as well as a versatile adhesive for mimicking natural photosynthesis. This work demonstrates that PDA accelerates the rate of photoinduced electron transfer from light‐harvesting molecules through two‐electron and two‐proton redox‐coupling mechanism. The introduction of PDA as a charge separator significantly increased the efficiency of photochemical water oxidation. Furthermore, simple incorporation of PDA ad‐layer on the surface of conducting materials, such as carbon nanotubes, facilitated fast charge separation and oxygen evolution through the synergistic effect of PDA‐mediated proton‐coupled electron transfer and the high conductivity of the substrate. Our work shows that PDA is an excellent electron acceptor as well as a versatile adhesive; thus, PDA constitutes a new electron gate for harvesting photoinduced electrons and designing artificial photosynthetic systems.