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Hybrid organic-inorganic heterogeneous catalytic interfaces, where traditional catalytic materials are modified with self-assembled monolayers (SAMs), create promising features to control a wide range of catalytic processes through the design of dual organic-inorganic active sites and induced confinement effect. To provide a fundamental insight, we investigated CO2 electroreduction into valuable C2 chemicals (CO2RR-to-C2) over SAMs-modulated Cu. Our theoretical results show that 1/4 monolayer aminothiolates improve the stability, activity and selectivity of CO2RR-to-C2 by: (1) decreasing surface energy to suppress surface reconstruction; (2) facilitating CO2 activation and C-C coupling through dual organic-inorganic (i.e., -NH, Cu) active sites; (3) promoting C-C coupling via confinement effects that enlarge the adsorption energy difference between CO and COH; (4) inducing local electric fields to Cu surface and changing its dipole moment and polarizability to be in favor of C-C coupling under electrode/electrolyte interfacial electric field.