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Electrochemical reduction of CO 2 to multi-carbon products is very attractive yet particularly challenging due to the low efficiency of C-C coupling over currently used electrocatalysts. In this work, we report a dual-atom catalyst (Cu 2 /NC) capable of selectively promoting electro-reduction of CO 2 to C 2 H 4. The Faradaic efficiency of CO 2 -to-C 2 H 4 over the Cu 2 /NC is up to ∼34.9% with a current density of 33.6 mA·cm−2. By contrast, its Cu single-atom counterpart only generates CO without forming C 2 H 4. The density functional theory (DFT) calculations reveal that the Cu-Cu sites largely promote the adsorption of *CO and reduce the energy barrier of C-C coupling between the adsorbed *CO relative to that of the single Cu sites, which accounts for the high C 2 H 4 selectivity of the Cu 2 /NC. [Display omitted] • Highly efficient Cu dual-atom catalysts were prepared to catalyze CO2RR. • Compared with Cu single-atom catalyst, dual-atom catalyst was more favorable to reduce CO2 to multi-carbon product C2H4. • DFT calculations revealed that the energy barrier of C-C coupling was largely reduced on the dual Cu catalysts. [ABSTRACT FROM AUTHOR]