A　variety　of　MgAl-layered　double　hydrotalcites　(MA-LDHs-x)　with　different　Mg/Al　molar　ratios　(1 : 3-5 : 1)　were　prepared　by　a　novel　solid-thermal　approach.　The　obtained　MA-LDH-x　catalysts　were　characterized　by　various　techniques.　These　results　confirm　the　successful　preparation　of　MA-LDHs-x　with　a　high　degree　of　crystallinity,　large　BET　surface　areas,　and　unique　nanosheet　structures　with　controllable　hexagonal　morphology.　In　addition,　MA-LDHs-x　possess　tunable　OH-　group　contents,　which　could　be　correlated　with　the　molar　ratio　of　Mg/Al.　As　a　result,　the　MA-LDH-x　catalysts　exhibited　better　catalytic　performance　in　carbonyl　sulfide　(COS)　hydrolysis　(COS　conversion:　100%　at　130　°C　for　MA-LDHs-3 : 1　vs.　38%　at　130　°C　for　commercial　Fe2O3)　and　H2S　selective　oxidation　(H2S　conversion:　100%　at　150　°C　for　MA-LDHs-3 : 1　vs.　41%　at　150　°C　for　commercial　Fe2O3)　than　commercial　desulfurization　catalysts.　Superior　activities　found　in　MA-LDH-x　catalysts　were　attributed　to　their　controllable　2D　nanosheet　structures,　and　the　unique　structural　characteristics　enhance　the　mass　transfer　of　guest　molecules.　Notably,　the　exposed　OH-　base　sites　of　MA-LDHs-x　efficiently　activate　the　acid　COS　and　H2S,　which　facilitate　the　COS　hydrolysis　to　H2S,　and　the　selective　H2S　oxidation　to　elemental　sulfur.　©　The　Royal　Society　of　Chemistry　and　the　Centre　National　de　la　Recherche　Scientifique.