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Solar-driven conversion of bicarbonate (HCO3−) to carbonaceous fuels and/or chemicals provides an alternative route for the development of sustainable carbon economies. However, promoting the HCO3− reduction rate and tuning product selectivity remain significant challenges. This study reports the identification of isolated Ni/Cu atomic pairs dispersed on a BiOCl surface (Ni1/Cu1-BOC) as a promising candidate for efficient HCO3− reduction under UV-vis light irradiation. The optimized photocatalyst exhibits a high CO formation rate of 157.1 μmol g−1 h−1 with nearly 100% selectivity, even in the absence of added proton sources, sacrificial agents, or sensitizers. Experimental and theoretical investigations reveal that the atomically dispersed Ni/Cu pairs facilitate the protonation of HCO3− to CO2, which then undergoes a H+-assisted reduction pathway to produce CO, with *COOH as the intermediate. The synergistic effects of the Ni/Cu atomic pairs simultaneously promote the HCO3−-to-CO2 conversion and the subsequent CO2-to-CO reduction, providing valuable insights for the development of efficient diatomic catalysts for photocatalytic HCO3− reduction reactions. [ABSTRACT FROM AUTHOR]