As　a　class　of　natural　clay　minerals,　the　special　surface　characteristic　of　the　negatively　charged　outer　surface　and　the　positively　charged　inner　lumen　enables　halloysite　to　be　of　potential　interest　for　catalytic　applications.　In　this　work,　thermal　treatment　and　modification　with　cetyltrimethylammonium　bromide　made　the　outer　surface　of　halloysite　hydrophobic,　which　resulted　in　the　selective　loading　of　palladium　on　the　hydrophilic　inner　surface　of　halloysite.　The　designed　site-oriented　loading　endowed　catalysts　with　the　desired　structure　and　favorable　properties　for　methane　combustion.　Because　of　the　uniformly　dispersed　palladium　particles　(ca.　2　nm),　a　suitable　ratio　of　Pd2+/Pd4+,　better　reducibility,　and　appropriate　surface　acidity,　the　tailored　catalyst　exhibited　a　remarkably　higher　activity　with　the　T99　decreasing　from　620　°C　(unmodified　catalysts)　to　425　°C.　More　importantly,　the　stabilized　palladium　species　could　resist　sintering　and　the　diminishing　of　hydroxyl　groups　on　the　surface　weakened　the　interaction　with　water,　invoking　an　excellent　long-term/cyclic　stability　and　water　resistance　for　methane　combustion.　Copyright　©　2020　American　Chemical　Society.