Polymer-based ZnO/TiO2 NCs flexible sheets with high dielectric permittivity and low loss factor have numerous applications in light emitting and energy storage devices. In this work, polymer-based ZnO/TiO2 NCs are synthesized by co-precipitation technique. The development of various diffraction planes (X-rays diffraction analysis) related to TiO2 and ZnO phases confirms the synthesis of polycrystalline polymer-based ZnO/TiO2 NCs. The crystallinity of various phases is associated with increasing ZnO nanofillers. The surface morphology (scanning electron microscopic analysis) comprising of nanoparticles of different shapes is associated with increasing amount of nanofillers. The EDX analysis confirms the presence of Zn, O and Ti in the synthesized polymer-based ZnO/TiO2 NCs. Dielectric measurements demonstrating the sharp increase in dielectric permittivity with relatively low dissipation factor of synthesized polymer-based ZnO/TiO2 NCs are associated with increasing amount of ZnO nanofillers. The static value of dielectric constant (e’) at low frequency (100 Hz) is found to be 14.56 for sample having 10% ZnO nanofillers that is 2.11 times greater than pure PVDF and it shows relatively low value of dissipation factor. The observed σac of synthesized polymer-based ZnO/TiO2 NCs at 3.0×105 Hz and 1.0×106 Hz are ranged from 3.75-9.79 and 15.61-42.72 mS/m respectively. The decreasing complex impedance and increasing electric modulus further confirm that the synthesized polymer-based ZnO/TiO2 NCs flexible sheets are the promising candidate for better capacitive performance showing high strength and flexibility.