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ZSM-5 nanosheets were prepared using [C₁₈H₃₇-N⁺(CH₃)₂-C₆H₁₂-N⁺(CH₃)₂-C₆H₁₃]Br₂ as a template and then ion-exchanged with Cu cations. The catalytic performance of the obtained Cu-ZSM-5 nanosheets in N₂O decomposition was investigated and compared with that of conventional Cu-ZSM-5. Higher activity as well as better stability was observed for Cu-ZSM-5 nanosheets although the Cu contents of the catalysts were identical. Relevant characterization was conducted using XRF, ICP, XRD, N₂ adsorption–desorption, SEM, TEM, CO-IR, H₂-TPR and O₂-TPD. The data show that the better catalytic performance of Cu-ZSM-5 nanosheets is probably due to better accessibility of active sites, better reducibility of active Cu⁺ species, and the weakened interaction between oxygen and Cu⁺ sites.