It　is　imperative　to　explore　advanced　catalysts　that　could　activate　methane　in　a　mild　manner.　Herein,　using　density　function　theory　(DFT),　we　have　investigated　the　activation　mechanism　for　the　dissociation　of　methane,　which　is　adsorbed　on　the　triangle　defect　surface　of　ZnO@Au,　where　the　defect　ZnO(0　0　1)　nanosheet　is　supported　by　Au(1　1　1).　We　found　that　the　triangle　defects　induced　coordination　unsaturated　O　and　Zn　on　the　ZnO@Au　are　of　great　importance　for　this　dissociation　process,　as　the　coordination　unsaturated　O　and　Zn　not　only　can　stabilize　the　methane,　but　also　can　polarize　the　C[sbnd]H　bond　through　the　dynamic　frustrated　Lewis　pairs.　Compared　with　perfect　ZnO@Au　heterojunction,　the　defect　ZnO@Au　can　activate　methane　via　precursor-mediated　mechanism　where　the　activation　energy　(0.21　eV)　is　lower　than　the　absolute　value　of　adsorption　energy　(0.48　eV).　Such　outstanding　activation　mainly　originates　from　the　electronic　interaction　between　the　methane　and　the　coordination　unsaturated　O　as　well　as　Zn.　Overall,　the　result　not　only　provide　a　vital　insight　into　the　catalytic　mechanism　of　the　methane　activation　on　ZnO@Au,　but　also　give　a　new　thought　to　develop　catalysts　for　the　facile　methane　activation.　©　2021　Elsevier　B.V.