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A highly active low-temperature MnOx wrapped cubic CeO2 (Ce@Mn) catalyst has been developed for the selective catalytic reduction of NOx by NH3. This core-shell catalyst exhibited over 90% NOx conversion at 100–300 °C, and also displayed high tolerance to H2O and SO2, which outperformed CeMn particles prepared via the co-precipitation method. The improved performance of Ce@Mn catalyst can be related to the presence of more Ce3+ and oxygen vacancies, which generate more surface chemisorbed oxygen. In-situ DRIFTS revealed that the reduction of NOx over Ce@Mn catalyst proceeded via the Langmuir-Hinshelwood (L-H) mechanism.