In order to enhance dielectric properties and energy storage density of poly(vinylidene fluoride-hexafluoro propylene) (PVDF-HFP), surface charged gas-phase Al2O3 nanoparticles (GP-Al2O3, with positive surface charges, epsilon' approximate to 10) are selected as fillers to fabricate PVDF-HFP-based composites via simple physical blending and hot-molding techniques. The results show that GP-Al2O3 are dispersed homogeneously in the PVDF-HFP matrix and the existence of nanoscale interface layer (matrix-filler) is investigated by SAXS. The dielectric constant of the composites filled with 10 wt % GP-Al2O3 is 100.5 at 1 Hz, which is 5.6 times higher than that of pure PVDF-HFP. The maximum energy storage density of the composite is 4.06 J cm(-3) at an electrical field of 900 kV mm(-1) with GP-Al2O3 content of 1 wt %. Experimental results show that GP-Al2O3 could induce uniform fillers' distribution and increase the concentration of electroactive beta-phase as well as enhance interfacial polarization in the matrix, which resulted in enhancements of dielectric constant and energy storage density of the PVDF-HFP composites. This work demonstrates that surface charged inorganic-oxide nanoparticles exhibit promising potential in fabricating ferroelectric polymer composites with relatively high dielectric constant and energy storage. (c) 2019 Wiley Periodicals, Inc. J. Polym. Sci., Part B: Polym. Phys. 2019, 57, 574-583