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We report single-atom Cu catalysts dispersed on nitrogen-doped carbon by a nitrogen-coordination strategy. The presence of nitrogen enabled good dispersion and attachment of atomic Cu species on the nitrogen-doped carbon frameworks with Cu–N_x configurations. The Cu doping concentrations and Cu–N_x configurations were well-tuned by the pyrolysis temperature. At a high Cu concentration of 4.9%_mol, the distance between neighboring Cu–N_x species was close enough to enable C–C coupling and produce C₂H₄. In contrast, at Cu concentrations lower than 2.4%_mol, the distance between Cu–N_x species was large so that the electrocatalyst favored the formation of CH₄ as C₁ products. Density functional theory calculations further confirmed the capability of producing C₂H₄ by two CO intermediates binding on two adjacent Cu–N₂ sites, while the isolated Cu–N₄, the neighboring Cu–N₄, and the isolated …