Piezopolymer poly(vinylidene fluoride-trifluoroethylene) (PVDF-TrFE) films doped with BaTiO3 (BT) and polydopamine coated BT (BT-Pdop) nanoparticles were prepared by spin-coating method. Polydopamine modifies the interfaces of inorganic BT nanoparticles and PVDF-TrFE matrix with its polar hydroxyl groups, enhancing the piezoelectric beta-phase. BT-Pdop nanoparticles were obtained in pH 8.5 buffer solution. For ferroelectric PVDF-TrFE, the favorable piezoelectric property comes from its ferroelectricity. Therefore, we studied the ferroelectric property of the nanocomposite films. The nanocomposite thin films possess better ferroelectric property than the pure PVDF-TrFE thin films, as demonstrated by the ferroelectric hysteresis curves. The remanent polarizations are 13.59 and 13.94 mu C/cm(2) after the doping of 1.0 wt% BT and 1.0 wt% BT-Pdop, respectively, which are about twice that of neat PVDF-TrFE. The piezoelectric beta-ferroelectric phase increases with doping, according to X-Ray Diffraction analysis. In addition, the images of polarized optical microscopy and atomic force microscopy also reveal significant enhancement in crystallinity. The neat PVDF-TrFE is a semicrystalline polymer and the size of crystalline spherulites increases with the addition of BT and BT-Pdop nanoparticles. However, even the crystallinity of PVDF-TrFE considerably improved with polydopamine interfacial modification of BT, the increase of remanent polarization due to Pdop is only marginal. We infer that there are other defects at interfaces of BT-Pdop doped PVDF-TrFE nanocomposites which counteract the beneficial effect of the polar OH of polydopamine. Considerable enhancement on ferroelectric property of BT-Pdop doped PVDF-TrFE nanocomposites is expected after these issues are addressed.