Electrocatalytic conversion of NO-to-NH3 holds immense potential for removing contaminants and producing zero-carbon fuel. To facilitate widespread commercial adoption of this technology, electrocatalysts with exceptional stability, high activity, and selective performance are urgently desired. We developed a novel dual-atom electrocatalyst, Fe–Mo@NG, in which Fe–Mo dimer is anchored to N-doped graphite. Through the first principle calculations, it is discovered that Fe–Mo@NG provided exceptional performance in NO-to-NH3 conversion. The parallel adsorption type was found can maximize the activation of NO. And the most favorable adsorption structure exhibits a limiting potential of −0.26 eV, surpassing that of most conventional electrocatalysts. The remarkable NORR activity of Fe–Mo@NG is traced back the synergistic effect between the dual-atom active site and the electronic interactions between the active site and NO. At high coverages, the interaction between intermediates and free NO molecules may lead to the formation of N2 or N2O. Overall, our research introduces a promising dual-atom electrocatalyst with broad applicability in NO reduction reactions, providing novel insights into the dual-atom catalysts design.