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The electrochemical reduction of CO2 could play an important role in addressing climate-change issues and global energy demands as part of a carbon-neutral energy cycle. Single-atom catalysts can display outstanding electrocatalytic performance; however, given their single-site nature they are usually only amenable to reactions that involve single molecules. For processes that involve multiple molecules, improved catalytic properties could be achieved through the development of atomically dispersed catalysts with higher complexities. Here we report a catalyst that features two adjacent copper atoms, which we call an 'atom-pair catalyst', that work together to carry out the critical bimolecular step in CO2 reduction. The atom-pair catalyst features stable Cu-1(0)-Cu-1(x+) pair structures, with Cu-1(x+) adsorbing H2O and the neighbouring Cu-1(0) adsorbing CO2, which thereby promotes CO2 activation. This results in a Faradaic efficiency for CO generation above 92%, with the competing hydrogen evolution reaction almost completely suppressed. Experimental characterization and density functional theory revealed that the adsorption configuration reduces the activation energy, which generates high selectivity, activity and stability under relatively low potentials.