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Abstract The effect of rare earth (RE) single atoms on photocatalytic activity is very complex due to its special electronic configuration, which leads to few reports on the RE single atoms. Here, Dy³⁺single atom composite photocatalysts are successfully constructed based on both the special role of Dy³⁺and the special advantages of CdS/g‐C₃N₄heterojunction in the field of photocatalysis. The results show that an efficient way of electron transfer is provided to promote charge separation, and the dual functions of CO₂molecular activation of rare‐earth single atom and 4flevels as electron transport bridge are fully exploited. It is exciting that under visible‐light irradiation, the catalytic performance of CdS:Dy³⁺/g‐C₃N₄is≈6.9 times higher than that of pure g‐C₃N₄. The catalytic performance of CdS:Dy³⁺and CdS:Dy³⁺/g‐C₃N₄are≈7 and≈13.7 times higher than those of pure CdS, respectively. Besides, not all RE ions are suitable for charge transfer bridges, which is not only related to the 4flevels of RE ions but also related to the bandgap structure of CdS and g‐C₃N₄. The pattern of combining single‐atom catalysis and heterojunction opens up new methods for enhancing photocatalytic activity.