The design of the controlled coordination environment over Cu sites for selective catalytic reduction of NOx using NH3 as reductant (NH3‐SCR) is still challenging. A series of dispersed Cu catalysts with different coordination environments were prepared by metal‐template/metal‐ion exchanged method and random grafting method. Meanwhile, their NH3‐SCR catalytic performance was explored. The catalyst C/T9‐M, prepared through metal‐template/metal‐ion exchanged method, achieved relatively good activity with the NOx conversion of ~100% in the temperature region of 250°C°C–400°C. It was ascribed to C/T9‐M containing a higher amount of the isolated Cu2+ and without occurring the direct oxidation of NH3 to NO at high temperature. On the contrary, C/T9‐R synthesized using random grafting method demonstrated more outstanding NH3‐SCR performance with the NOx conversion of ~100% in the temperature region of 200°C°C–350°C due to more [Cu(OH)]+. Our experimental results confirmed that the active [Cu(OH)]+ was capable of facilitating the low‐temperature activity for NH3‐SCR and the isolated Cu2+ facilitates NOx conversion under high temperature. In addition, compared with the C/T9‐R catalyst, the C/T9‐M catalyst had less Cu loading, which laterally proved that controlling the coordination environment of Cu sites could effectively improve the NH3‐SCR performance under high temperature. What's more, C/T9‐M had more glorious the resistance of H2O and SO2 than C/T9‐R. This work furnishes reformatory pathway for the invention of noticeable NH3‐SCR catalysts. It is expedient for academic and practical applications in the future.
