Summary: The development of a novel technique for the preparation of homogeneous BaTiO3/polyvinylidene fluoride (BT/PVDF) nanocomposites without obvious agglomeration of BaTiO3 particles was reported in this communication. The morphology, structure, and frequency dependence of the dielectric properties of the nanocomposites were characterized. All results show that the dielectric properties of the nanocomposites in this study are desirable, and the process for preparing the nanocomposites has potential applications in the electronic industry.