Flexible polymer hybrid nanocomposites were fabricated by a simple phase separation method. Barium titanate (BT NPs) and carbon nanotubes (MWCNTs) were dispersed homogeneously in the PVDF polymer matrix. A high real permittivity (71.7) and a low dielectric loss (0.045) were achieved with 37.1 vol % BT NPs and 3 vol % MWCNT. The breakdown strength was improved by annealing heat treatments. An equivalent circuit model was proposed to account for the different components in the nanocomposite. Finite element simulations were conducted for quantitative analysis and improved predictability of the properties.