Hydrogen　sulfide　(H2S)　is　highly　toxic　and　corrosive,　and　its　selective　removal　from　fuel　and　flue　gases　is　of　significance.　It　is　a　challenge　to　develop　a　dual-role　material　for　efficient　H2S　capture　as　well　as　selective　H2S　oxidation.　In　the　present　work,　we　designed　a　class　of　nitrogen-decorated　ordered　mesoporous　carbon　spheres　(denoted　herein　as　N-OMCS-T,　where　T　stands　for　carbonization　temperature)　for　such　an　end.　The　N-OMCS-T　with　ordered　mesopores　are　large　in　BET　surface　area　(1201-1500　m2/g),　and　enriched　with　nitrogen　sites　of　pyridinic　and　pyrrolic　nature,　and　exhibit　strong　interaction　with　H2S　as　verified　in　DFT　calculations.　With　large　BET　surface　areas,　ordered　mesopores,　and　abundant　nitrogen　sites,　the　N-OMCS-T　materials　show　extraordinary　efficacy　for　the　capture　of　H2S:　H2S　capacities　are　up　to　13.4　mmol/g　(0　°C,　1　bar),　and　the　Ideal　Adsorption　Solution　Theory　selectivity　in　cases　of　H2S/CO2,　H2S/CH4,　and　H2S/N2　is　2.1-8.5,　11.0-25.5,　and　30.4-81.7,　respectively,　much　higher　than　those　of　porous　materials　such　as　activated　carbon,　OMCS,　Zeolite　A,　UiO-66,　and　SBA-15.　Moreover,　N-OMCS-T　could　act　as　efficient　and　long-lived　metal-free　catalysts　for　selective　oxidation　of　the　captured　H2S　to　sulfur　under　mild　conditions.　©　Copyright　2019　American　Chemical　Society.