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A catalyst system with dedicated selectivity toward a single hydrocarbon or oxygenate product is essential to enable the industrial application of electrochemical conversion of CO₂ to high-value chemicals. Cu is the only known metal catalyst that can convert CO₂ to high-order hydrocarbons and oxygenates. However, the Cu-based catalysts suffer from diverse selectivity. Here, we report that the functionalized graphene quantum dots can direct CO₂ to CH₄ conversion with simultaneous high selectivity and production rate. The electron-donating groups facilitate the yield of CH₄ from CO₂ electro-reduction while electron-withdrawing groups suppress CO₂ electro-reduction. The yield of CH₄ on electron-donating group functionalized graphene quantum dots is positively correlated to the electron-donating ability and content of electron-donating group. The graphene quantum dots functionalized by either –OH or –NH₂ …