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With the rapid development of modern society and the chemical industry, the demand for hydroxylamine (NH2OH) has expanded significantly across diverse fields. However, its conventional synthesis remains challenged by severe pollution and intensive resource consumption. Building upon the experimentally realized Fe@N4 structure, we propose a ligand coordination strategy to module the electronic structure of iron single-atom catalysts via 15 axial ligands (-F, -Cl, -Br, -I, -N, -O, −OH, -OOH, −CH, −CH2, −CH3, -NH2, -SH, −CN, -SCH3), aiming to enhance the electrocatalytic reduction of nitric oxide (NO) to NH2OH. Among these, 13 catalysts effectively suppress hydrogen evolution reactions and the generation of undesired byproducts such as NH3 and N2O/N2. Notably, the −CH2 ligand significantly alters the local electronic environment of the active site, enabling the activation of NO molecules through an electronic “accept-donate” mechanism. This modulation enhances both the activity and selectivity for NO reduction, ultimately leading to a spontaneous, exothermic conversion of NO to NH2OH. This work theoretically proposes a strategy whereby axial coordination can enhance the catalytic reactivity of single-atom catalysts.