The simultaneous achievement of efficient NOx reduction and N2O byproduct suppression during NH3-SCR represents a core challenge in engine exhaust aftertreatment. This study prepared Co-Fe-Beta zeolite via an impregnation method. Combining characterization, catalytic evaluation and density functional theory (DFT) calculations, we systematically investigated the catalyst''s microstructure, catalytic performance and reaction mechanism. Characterization results demonstrate that no large metal oxide particles or agglomeration are observed in the Co-Fe-Beta zeolite catalysts. Co and Fe atoms are uniformly dispersed within the nanopores of the Beta zeolite framework, while the characteristic crystalline phase, nanoporous structure of the Beta zeolite are well preserved. Catalytic evaluation indicates that 2 %-2 %-Co-Fe-Beta exhibits optimal performance in a 100400 degrees C venting atmosphere, demonstrating significantly enhanced N2 selectivity compared to single-component Fe-Beta and substantially reduced N2O by-product formation. DFT calculations reveal that the Fast-SCR main reaction follows the Eley-Rideal (E-R) mechanism, with the pathway ''dual NH3 adsorption -> NO activation to form N2H intermediate -> NO2 participation in reaction'' (Path1) being the dominant route, exhibiting a ratedetermining step energy barrier of merely 0.50 eV. The synergistic effect between Co and Fe not only affords excellent NOx reduction performance in NH3-SCR but also achieves effective suppression of N2O byproduct formation. This study confirms the crucial role of the synergistic effect between Co and Fe bimetallic sites in boosting NH3-SCR catalytic activity and N2 selectivity while suppressing N2O byproduct formation. It provides experimental evidence and theoretical guidance for the development of high-performance exhaust aftertreatment catalysts.