Selective　removal　of　carbonyl　sulfide　(COS)　and　hydrogen　sulfide　(H2S)　is　the　key　step　for　natural　gas　desulfurization　due　to　the　highly　toxic　and　corrosive　features　of　these　gaseous　sulfides,　and　efficient　and　stable　desulfurizers　are　urgently　needed　in　the　industry.　Herein,　we　report　a　class　of　nitrogen-functionalized,　hierarchically　lamellar　carbon　frameworks　(N-HLCF-xs),　which　are　obtained　from　the　structural　transformation　of　Zn　zeolitic　imidazolate　frameworks　via　controllable　carbonization.　The　N-HLCF-xs　possess　the　desirable　characteristics　of　large　Brunauer-Emmett-Teller　surface　areas　(645-923　m2/g),　combined　primary　three-dimensional　microporosity　and　secondary　two-dimensional　lamellar　microstructure,　and　high　density　of　nitrogen　base　sites　with　enhanced　pyridine　ratio　(17.52　wt　%,　59.91%).　The　anchored　nitrogen　base　sites　in　N-HLCF-xs　show　improved　accessibility,　which　boosts　their　interaction　with　acidic　COS　and　H2S.　As　expected,　N-HLCF-xs　can　be　employed　as　multifunctional　and　efficient　desulfurizers　for　selective　removal　of　COS　and　H2S　from　natural　gas.　COS　was　first　transformed　into　H2S　via　catalytic　hydrolysis,　and　the　produced　H2S　was　then　captured　and　separated　and　catalyzed　oxidation　into　elemental　sulfur.　The　above　continuous　processes　can　be　achieved　with　solo　N-HLCF-xs,　giving　extremely　high　efficiencies　and　reusability.　Their　integrated　desulfurization　performance　was　better　than　many　desulfurizers　used　in　the　area,　such　as　activated　carbon,　β　zeolite,　MIL-101(Fe),　K2CO3/γ-Al2O3,　and　FeOx/TiO2.　©　2022　The　Authors.　Published　by　American　Chemical　Society.