High overall performance, including high dielectric constant, low loss, high breakdown strength, fine flexibility, and strong tensile properties, is difficult to achieve simultaneously in polymer nanocomposites. In our prior work, we modified the surfaces of alpha-SiC nanoparticles and chemically cross-linked the polymeric matrix to simultaneously promote the dielectric and mechanical properties of composites. In this work, a novel strategy of high-temperature plastification towards a polymeric matrix has been proposed to fabricate ternary nanocomposites with balanced dielectric and mechanical characteristics by the solution cast method in order to reduce costs and simplify steps during large-scale preparation. Poly(vinylidene fluoride-chlorotrifluoroethylene) with inner double bonds as matrix, unfunctionalized alpha-SiC nanoparticles (NPs) as filler, and dibutyl phthalate (DBP) as plasticizer were employed. By introducing DBP and high-temperature treatment, the dispersion of NPs and the degree of compactness of the interface regions were both improved due to the reduced cohesion of the fluoropolymer, resulting in an increase in the dielectric constant (by 30%) and breakdown strength (by 57%) as well as the lowering of loss (by 30%) and conductivity (by 16%) in nanocomposites. Moreover, high-temperature plastification contributed to the promotion of flexible and tensile properties. This work might open the door to large-scale fabrication of nanocomposite dielectrics with high overall properties through the cooperation of the plasticizer and high temperature.