We report on the application of cold atmospheric-pressure plasmas to modify silica nanoparticles to enhance their compatibility with polymer matrices. Thermally nonequilibrium atmospheric-pressure plasma is generated by a high-voltage radio frequency power source operated in the capacitively coupled mode with helium as the working gas. Compared to the pure polymer and the polymer nanocomposites with untreated SiO(2), the plasma-treated SiO(2)-polymer nanocomposites show higher dielectric breakdown strength and extended endurance under a constant electrical stress. These improvements are attributed to the stronger interactions between the SiO(2) nanoparticles and the surrounding polymer matrix after the plasma treatment. Our method is generic and can be used in the production of high-performance organic-inorganic functional nanocomposites.