A　cofunctionalized　silica-supported　palladium　catalyst　has　been　successfully　designed　and　controllably　fabricated　for　the　selective　hydrogenation　of　nitrile　butadiene　rubber　(NBR).　The　amino　groups　on　the　surface　can　anchor　and　stabilize　Pd　particles　via　the　strong　coordination　with　diamine　ligands　and　methyl　groups　can　enhance　surface　hydrophobicity,　weakening　the　adhesion　of　NBR/hydrogenated　NBR　on　catalyst　and　accelerating　the　desorption　of　product　to　re-expose　the　active　sites.　The　cofunctionalized　catalyst　with　small-sized　and　well-dispersed　Pd　particles　exhibits　an　enhanced　activity　and　stability,　which　can　be　easily　recycled　by　filtration　and　reused　without　any　treatment.　It　remains　a　high　activity　and　100%　selectivity　to　C=C　after　recycling　five　times,　and　only　a　slight　loss　of　Pd　is　detected　in　products.　Such　catalyst　with　cofunctionalized　surface　is　very　efficient　for　NBR　hydrogenation　and　also　can　be　applied　to　other　catalytic　systems　to　tune　their　selectivity,　activity,　and　reusability.　©　2019　American　Chemical　Society.