A　core-shell　inorganic/polymer　materials　with　abundant　compositions　and　multiple　shapes　have　attracted　many　attentions　recently　for　their　harmonious　interfacial　compatibility,　high　dielectric　performance,　and　thereby　the　prospect　of　applications　in　energy　storage　devices.　In　this　work,　for　improving　the　interfacial　compatibility　of　in　organiclpolymer　nanocomposites,　the　BaTiO3　(BT)　nano-powders　are　coated　successively　by　using　double　shell　polyamide　(HBP)　and　dopamine　(PDA)　that　is　decorated　with　nanoscale　Ag　particles.　In　addition,　a　P(VDF-CTFE)　with　high　breakdown　electric　field　and　proper　dielectric　permittivity　are　selected　as　the　polymer　matrix,　and　the　flexible　0-3　nanocomposite　of　Ag　decorated　P(VDF-CTFE)/BT@HBP@PDA　films　with　20μm　in　thickness　are　obtained　through　spin-casting　method.　The　morphologies　from　FESEM　show　that　the　interface　between　BaTiO3　and　P(VDF-CTFE)　has　been　improved　significantly　and　BaTiO3　is　homogeneous　dispersion　in　the　polymer　matrix.　Consequently,　the　multicomponent　nanocomposites　possess　the　large　dielectric　permittivity　(ϵr40)　and　a　low　dielectric　loss　tangent　(0.1　Hz)　since　the　ionic　polarization　of　BaTiO3　and　the　penetration　effect　of　electrons.　The　result　provides　an　effective　way　of　interfacial　improving　that　through　various　mutual　promoting　mediums　to　achieve　high　dielectric　performance　composite　materials　for　their　potential　applications　in　energy　storage　areas.　©　2018　IEEE.