Single‐atom photocatalysis has been demonstrated as a novel strategy to promote heterogeneous reactions. There is a diversity of monoatomic metal species with specific functions; however, integrating representative merits into dual‐single‐atoms and regulating cooperative photocatalysis remain a pressing challenge. For dual‐single‐atom catalysts, enhanced photocatalytic activity would be realized through integrating bifunctional properties and tuning the synergistic effect. Herein, dual‐single‐atoms supported on conjugated porous carbon nitride polymer are developed for effective photocatalytic CO2 reduction, featuring the function of cobalt (Co) and ruthenium (Ru). A series of in situ characterizations and theoretical calculations are conducted for quantitative analysis of structure–performance correlation. It is concluded that the active Co sites facilitate dynamic charge transfer, while the Ru sites promote selective CO2 surface‐bound interaction during CO2 photoreduction. The combination of atom‐specific traits and the synergy between Co and Ru lead to the high photocatalytic CO2 conversion with corresponding apparent quantum efficiency (AQE) of 2.8% at 385 nm, along with a high turnover number (TON) of more than 200 without addition of any sacrificial agent. This work presents an example of identifying the roles of different single‐atom metals and regulating the synergy, where the two metals with unique properties collaborate to further boost the photocatalytic performance.

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