Atomic Printing Strategy Achieves Precise Anchoring of Dual‐Copper Atoms on C2N Structure for Efficient CO2 Reduction to Ethylene

Abstract Isolated metal sites catalysts (IMSCs) play crucial role in electrochemical CO 2 reduction, with potential industrial applications. However, tunable synthesis strategies for IMSCs are limited. Herein, we present an atomic printing strategy that draws inspiration from the ancient Chinese “movable‐type printing technology”. Selecting customizable combinations of metal atoms as metal precursors from an extensive binuclear metal library. A series of dual‐atom catalysts were prepared by utilizing the edge nitrogen atoms in the C 2 N cavity as anchoring “pincers” to capture metal atoms. To prove utility, the dual atom catalyst Cu 2 ‐C 2 N is investigated as electrocatalytic CO 2 RR catalyst. The synergistic interaction of dual Cu atoms promotes C−C coupling and guarantees FE C2+ (90.8 %) and FE C2H4 . (71.7 %) at −1.10 V vs RHE. DFT calculations revealed the Cu 2 site would be subtly flipped during CO 2 RR for enhancing *CO adsorption and dimerization. We validate that atomic printing strategies are applicable to wide range of metal combinations, representing a significant advancement in the development of IMSCs.