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

Isolated metal sites catalysts (IMSCs) play crucial role in electrochemical CO2 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 form an extensive binuclear metal library. A series of dual‐atom catalysts were prepared by utilizing the edge nitrogen atoms in the C2N cavity as anchoring "pincers" to capture metal atoms. To prove utility, the dual atom catalyst Cu2‐C2N is investigated as electrocatalytic CO2RR catalyst. The synergistic interaction of dual Cu atoms promotes C‐C coupling and guarantees FEC2+ (90.8%) and FEC2H4. (71.7%) at ‐1.10 V vs RHE. DFT calculations revealed the Cu2 site would be subtly flipped during CO2RR 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.