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Abstract Copper-based catalyst is uniquely positioned to catalyze the hydrocarbon formations through electrochemical CO2 reduction. The catalyst design freedom is limited for alloying copper with H-affinitive elements represented by platinum group metals because the latter would easily drive the hydrogen evolution reaction to override CO2 reduction. We report an adept design of anchoring atomically dispersed platinum group metal species on both polycrystalline and shape-controlled Cu catalysts, which now promote targeted CO2 reduction reaction while frustrating the undesired hydrogen evolution reaction. Notably, alloys with similar metal formulations but comprising small platinum or palladium clusters would fail this objective. With an appreciable amount of CO-Pd1 moieties on copper surfaces, facile CO* hydrogenation to CHO* or CO-CHO* coupling is now viable as one of the main pathways on Cu(111) or Cu(100) to selectively produce CH4 or C2H4 through Pd-Cu dual-site pathways. The work broadens copper alloying choices for CO2 reduction in aqueous phases.