[en] The application of nickel in electrocatalytic reduction of CO₂ has been largely restricted by side reaction (hydrogen evolution reaction) and catalyst poisoning. Here we report a new strategy to improve the electrocatalytic performance of nickel for CO₂ reduction by employing a nitrogen-carbon layer for nickel nanoparticles. Such a nickel electrocatalyst exhibits high Faradaic efficiency 97.5% at relatively low potential of -0.61 V for the conversion of CO₂ to CO. Density functional theory calculation reveals that it is thermodynamically accomplishable for the reduction product CO to be removed from the catalyst surface, thus avoiding catalyst poisoning. Also, the catalyst renders hydrogen evolution reaction to be suppressed and hence reasonably improves catalytic performance. .