H2S　catalytic　elimination　via　selective　oxidation　process　has　received　considerable　attention　because　it　can　transform　highly　toxic　H2S　into　elemental　sulfur　under　mild　condition　without　thermodynamic　limitation.　For　this　purpose,　catalysts　with　high　performance　in　H2S　capture　and　selective　oxidation　are　urgently　needed.　Herein,　we　report　novel　nitrogen-doped　carbon-based　catalysts　(denoted　as　PPy-KOH-T),　which　are　synthesized　by　direct　carbonization　of　polypyrrole　at　600-800　°C　using　KOH　as　an　activator.　The　obtained　PPy-KOH-T　shows　large　specific　surface　areas　(1116-3157　m2/g),　hierarchical　structure,　and　abundant　nitrogen　active　sites.　As　a　result,　PPy-KOH-T　exhibits　high　performance　in　H2S　selective　capture.　The　H2S　adsorption　capacity　of　PPy-KOH-700　is　as　high　as　19.7　mmol/g　(0　°C,　1　bar),　and　the　ideal　adsorption　solution　theory　(IAST)　selectivity　of　H2S/N2　is　up　to　117.6,　which　is　much　better　than　that　of　activated　carbon　(4.8).　It　is　found　that　PPy-KOH-T　could　completely　catalyze　the　oxidation　of　H2S　into　elemental　sulfur　at　temperatures　as　low　as　150　°C.　It　can　be　applied　to　the　purification　of　high-sulfur　natural　gas　and　blast　furnace　gas　and　the　recovery　of　elemental　sulfur.　Significantly,　the　as-prepared　catalyst　displays　superior　long-term　stability　in　the　desulfurization　reaction　compared　with　g-C3N4　and　commercial　Fe2O3　©　2021　American　Chemical　Society