The development of efficient and stable nanocatalysts is crucial for the catalytic removal of H 2 S through selective oxidation to sulfur. Inspired by the different catalytic activity and selectivity of CeO 2 and MnO 2 for the reaction, cerium−manganese (Ce−Mn) nanocomposite oxides with tunable phase structure and unique surface properties were constructed to optimize the catalytic performance. By regulating the molar ratio of Ce and Mn components, a novel catalyst structure comprising Ce−Mn solid solution and amorphous CeO 2 is synthesized from Ce−Mn oxide with n Ce /n Mn ratio of 0.5 (50Ce−Mn). Compared with the unmodified MnO 2 , the tailored 50Ce−Mn possesses a high specific surface area, which facilitates the access of reactants to active sites and the desorption of formed sulfur. More importantly, strong Ce−Mn interaction and abundant surface-active oxygen species are generated, contributing to the regeneration of Mn 4+ /Ce 4+ active sites, facilitating the formation of sulfur, and inhibiting the accumulation of sulfates during the reaction. Consequently, 50Ce−Mn presents a superior catalytic activity (T 100 of 150 °C), stability, and sulfur selectivity even under relatively high weight hourly space velocity conditions (23,000 mL•g −1 •h −1 ). This study provides an example of how catalytic performance can be boosted through phase structure regulation on nanocomposites.