To further improve their energy storage density, adding high-dielectric-constant ceramic fillers into polymers has become a common method. In comparison with nanoparticle fillers, 1D and 2D nanofillers can greatly suppress the propagation of breakdown path in composite, and thus play a key role in rising the breakdown field and energy storage density of composite materials. However, the energy storage density in the organic/inorganic composites is largely limited as a result of the incompatibility between the interfaces of constituents. Here, DOPA was coated on the surface of Ti0.87O2 nanosheets, which was synthesized via liquid-phase exfoliation. DOPA@Ti0.87O2 nanofillers were employed to fabricate flexible poly(vinylidene fluoride. )(PVDF) films. The experimental results show that the energy storage efficiency of the resulting composite film is about 70%, about 17% higher than that of composite film filled with Ti0.87O2 (~60%).