Detoxicating　materials　of　chemical　warfare　agents　(CWAs)　and　their　simulants　play　a　critical　role　in　reducing　pollution　contamination　and　environmental　renovation.　In　this　work,　we　present　a　simple　strategy　to　prepare　a　core–shell　structure　Fe3O4/UiO-66-NH2/ILs@mSiO2　using　hydrogen　bonding　association　and　electrostatic　forces.　We　performed　disinfection　studies　on　dimethyl　4-nitrophenyl　phosphate　(DMNP)　and　2-chloroethyl　ethyl　sulfide　(2-CEES).　The　synergistic　effects　of　catalytic　activations　for　CWAs,　which　reduce　the　electron　transport　distance　and　lower　the　reaction　energy　barrier,　lead　to　an　increase　in　hydrolysis　and　Fenton-like　reactions　efficiency.　Eliminationing　tests　of　DMNP　and　2-CEES　showed　that　the　half-lives　of　the　degradation　reactions　were　128.36　and　1.12　min,　respectively,　and　the　degradation　efficiency　did　not　decrease　significantly　after　4　cycles.　This　new　type　of　structure　could　be　magnetically　separated　within　60　s　to　facilitate　material　recovery　and　reuse.　Moreover,　the　presence　of　a　mesoporous　silica　shell　made　the　catalyst　particles　to　become　biocompatible　and　environmentally　friendly.　The　degradation　pathways　of　the　intermediates　were　revealed　based　on　nuclear　magnetic　resonance　spectroscopy　(NMR),　gaschromatography-mass　spectrometry　(GC–MS)　and　density　functional　theory　(DFT)　calculations.　The　effective　combination　of　catalysts　provided　a　facile　strategy　for　developing　multi-effect　synergistic　catalysts　for　the　elimination　of　CWAs　and　other　pollutants.　©　2024　Elsevier　B.V.