Catalytic　elimination　of　highly　toxic　COS　and　H2S　from　industrial　resources　plays　a　crucial　role　in　terms　of　production　safety　and　environmental　protection.　We　report　here　novel　calcination　induced　self-assembly　concept　to　the　fast　synthesis　of　ordered　mesoporous　carbons　with　structural　base　N　sites　(A-N-OMC-Ts,　where　T　stands　for　carbonization　temperature)　without　using　any　solvent　and　catalysts.　The　A-N-OMC-Ts　show　large　BET　surface　areas　(∼1538　m2/g),　ordered　mesoporosity,　and　the　base　N　sites　exhibit　versatile　structures　(e.g.　pyridine　and　pyrrole,　2.03–3.77　wt%).　As　a　result,　A-N-OMC-Ts　show　excellent　activities　in　hydrolysis　of　COS　to　H2S,　and　the　H2S　can　be　efficiently　captured　(∼10.5　mmol/g,　0　°C,　1　bar,　IAST　selectivity　H2S/N2　=　4963,　75　°C)　and　oxidized　into　elemental　sulfur　by　A-N-OMC-Ts.　The　complete　elimination　of　COS　and　H2S　over　A-N-OMC-Ts　was　performed　at　ambient　conditions　(50　°C　for　COS;　150　°C　for　H2S,　and　Ea　=　32.29　kJ/mol),　much　better　than　that　of　g-C3N4　(150　°C,　H2S　conversion　<　10%,　Ea　=　42.11　kJ/mol).　These　performances　are　outstanding　among　the　metal-free　catalysts　reported　previously.　A　plausible　mechanistic　scenario　involves　the　synergistic　effect　of　pyridinic　and　pyrrolic　N　as　well　as　the　intermediate　H2O2　was　proposed　by　us.　Coupled　the　cleavage　of　H-S　bond　and　S　release　that　accelerate　the　desulfuration　rate.　©　2020　Elsevier　Ltd