Polymer/semiconductor-insulator nanocomposites can display high dielectric constants with a relatively low dissipation factor under low electric fields, and thus seem to promising for high energy density capacitors. Here, a novel nanocomposite films is developed by loading two-dimensional (2D) core-shell structure Bi2Te3@SiO2 nanosheets in the poly (vinylidene fluoride-hexafluoro propylene) (P(VDF-HFP)) polymer matrix. The 2D Bi2Te3 nanosheets were prepared through simple microwave-assisted method. The experimental results suggesting that the SiO2 shell layer between the fillers and polymer matrix could effectively improve the dielectric constant, dielectric loss, AC conductivity, and breakdown strength of composites films. The composite films load with 10 vol.% 2D Bi2Te3@SiO2 nanosheets exhibits a high dielectric constant of 70.3 at 1 kHz and relatively low dielectric loss of 0.058 at 1 kHz. The finite element simulation of electric field and electric current density distribution revealed that the SiO2 shell layer between the fillers and polymer matrix could effectively improve the energy loss, local electric field strength, and breakdown strength of composite films. Therefore, this work will provide a promising route to achieve high-performance capacitors.