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Electrochemical reduction of CO to value-added chemicals by using renewable electricity offers a promising strategy to deal with rising CO emission and the energy crisis. Single-site zinc-coordinated nitrogen-codoped graphene (Zn-N-G) catalyzes the electrochemical reduction of CO to CO. The Zn-N-G catalyst exhibits excellent intrinsic activity toward CO reduction, reaching a faradaic efficiency of 91 % for CO production at a low overpotential of 0.39 V. X-ray absorption fine structure and X-ray photoelectron spectroscopy both confirm the presence of isolated Zn-N moieties, which act as the key active sites for CO formation. DFT calculations reveal the origin of enhanced activity for CO reduction on Zn-N-G catalysts. This work provide further understanding of the active centers on transition metal-nitrogen-carbon (M-N-C) catalysts for electrochemical reduction of CO to CO.