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Conventional Cu-ZSM-5 and special Cu-ZSM-5 catalysts with diverse morphologies (nanoparticles, nanosheets, hollow spheres) were synthesized and comparatively investigated for their performances in the selective catalytic reduction (SCR) of NO to N2 with ammonia. Significant differences in SCR behavior were observed, and nanosheet-like Cu-ZSM-5 showed the best SCR performance with the lowest T50 of 130 °C and nearly complete conversion in the temperature range of 200-400 °C. It was found that Cu-ZSM-5 nanosheets [mainly exposed (0 1 0) crystal plane] with abundant mesopores and framework Al species were favorable for the formation of high external surface areas and Al pairs, which influenced the local environment of Cu. This motivated the preferential formation of active copper species and the rapid switch between Cu2+ and Cu+ species during NH3-SCR, thus exhibiting the highest NO conversion. In situ diffused reflectance infrared Fourier transform spectroscopy (DRIFTS) results indicated that the Cu-ZSM-5 nanosheets were dominated by the Eley-Rideal (E-R) mechanism and the labile nitrite species (NH4NO2) were the crucial intermediates during the NH3-SCR process, while the inert nitrates were more prone to generate on Cu-ZSM-5 nanoparticles and conventional one. The combined density functional theory (DFT) calculations revealed that the decomposition energy barrier of nitrosamide species (NH2NO) on the (0 1 0) crystal plane of Cu-ZSM-5 was lower than those on (0 0 1) and (1 0 0) crystal planes. This study provides a strategy for the design of NH3-SCR zeolite catalysts.