Deep　hydrogenation　of　dicyclopentadiene　resin　(DCPD　resin)　plays　an　important　role　in　enhancing　its　performance　and　broadening　its　applications.　However,　designing　suitable　catalysts　for　promoting　DCPD　resin　deep　hydrogenation　remains　a　challenge　due　to　the　high　steric　hindrance　and　abundant　unsaturated　bonds　in　DCPD　resin,　requiring　strong　binding　to　C=C　double　bonds.　We　herein　propose　a　strategy　for　simultaneously　constructing　highly-dispersed　Ni　particles　for　hydrogen　dissociation　and　interfacial　Ni0/Ni(OH)+　sites　for　C=C　adsorption　by　controlled　reduction　of　Ni　phyllosilicate　(Ni　PS).　The　catalyst,　after　reduction　at　400　°C,　demonstrated　balanced　ratio　between　Ni0　and　interfacial　Ni0/Ni(OH)+　sites,　and　achieved　a　hydrogenation　degree　of　99.8%　(TOF:　68.8　h−1)　while　maintaining　99.3%　efficiency　after　seven　consecutive　cycles.　Through　in-situ　DRIFTS　analysis　and　density　functional　theory　(DFT)　calculations,　it　is　confirmed　that　the　introduction　of　Ni0/Ni(OH)+　interfacial　sites　results　in　superior　activity　compared　to　pure　Ni0　or　unreduced　PS　due　to　optimized　charge　transfer　and　electronic　configuration.　This　work　not　only　establishes　a　simple　and　environmentally-friendly　approach　to　design　efficient　catalysts　for　polymer　hydrogenation,　but　also　provides　insights　into　the　mechanism　of　unsaturated　bond　hydrogenation　through　the　synergistic　effects　of　Ni0　and　Ni0/Ni(OH)+　interfacial　sites.　©　2025　Elsevier　B.V.