Improving　sulfur　resistance　of　palladium-based　catalysts　is　crucial　for　the　sustained　and　efficient　methane　combustion.　Herein,　the　surface　property　of　catalysts　was　rationally　tailored　to　tune　the　dynamic　behavior　of　sulfur　species　on　active　sites　and　supports,　which　was　qualitatively　and　quantitatively　studied　through　a　combination　of　in-situ　and　on-line　characterizations.　Results　reveal　that　the　content　of　accumulated　sulfur　species　in　catalysts　increased　linearly　(0.20–0.59　mmol　SO2·g−1)　with　the　rise　of　the　surface　basic　sites,　while　it　was　restrained　in　catalysts　with　high　surface　acidity.　The　zirconium　doped　alumina　supported　palladium　catalyst　exhibited　a　moderate　surface　acidity/basicity,　meanwhile　it　showed　an　excellent　catalytic　activity　in　the　presence　of　SO2　and　after　regeneration.　Its　enhanced　sulfur　resistance　derived　from　the　proper　interaction　between　supports　and　sulfur　species,　the　facile　decomposition　of　zirconium　sulfates,　the　suppressed　formation　of　surface/bulk　aluminum　sulfates,　as　well　as　the　effective　regeneration　of　PdO　phase.　The　established　quantitative　correlation　between　accumulated　sulfur　species,　surface　acidity/basicity　and　catalytic　performance　paves　the　way　to　develop　sulfur-resistant　palladium-based　catalysts　for　oxidation　reactions.　©　2022　Elsevier　B.V.