The　development　of　efficient　and　stable　nanocatalysts　is　crucial　for　the　catalytic　removal　of　H2S　through　selective　oxidation　to　sulfur.　Inspired　by　the　different　catalytic　activity　and　selectivity　of　CeO2　and　MnO2　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　CeO2　is　synthesized　from　Ce-Mn　oxide　with　n(Ce)/n(Mn)　ratio　of　0.5　(50Ce-Mn).　Compared　with　the　unmodified　MnO2,　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　Mn4+/Ce4+　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　degrees　C),　stability,　and　sulfur　selectivity　even　under　relatively　high　weight　hourly　space　velocity　conditions　(23,000　mL　center　dot　g(-1)center　dot　h(-1)).　This　study　provides　an　example　of　how　catalytic　performance　can　be　boosted　through　phase　structure　regulation　on　nanocomposites.