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In this paper, BaTiO 3 platelets are utilized for the first time to incorporate into polymer matrix for energy storage. To improve the dispersibility and compatibility of the BaTiO 3 platelets in the composites, a new type of fluoro-polymer poly{2,5-bis[(2,3,5,6-tetrafluoro-4-trifluoromethyl)oxycarbonyl]styrene} (PM7F) was designed for the first time to engineer the surface of BaTiO 3 platelets by surface-initiated reversible-addition-fragmentation chain transfer polymerization method. Each structural unit in the molecular chain of this novel modifier contained 14 fluorine atoms, resulting in effectively decreasing the surface energy of BaTiO 3 platelets. As a result, the BaTiO 3 platelets modified by PM7F were homogeneously dispersed in the polymer poly(vinylidene fluoride-trifluoroethylene-chlorofluoroethylene) (P(VDF-TrFE-CTFE)) matrix. The permittivities of the nanocomposites were significantly improved compared with the pure polymer matrix. The energy storage density of the nanocomposites was largely enhanced by adding the BaTiO 3 platelets. The discharged energy density of the nanocomposite with 15 vol% BaTiO 3 platelets was 1.26 J/cm 3 , which was nearly double to that of pure P(VDF-TrFE-CTFE) (0.64 J/cm 3 ) at the same electric field (60 kV/mm). The findings provide an effective modifier and a new routine for high performance capacitors. [ABSTRACT FROM AUTHOR]