The dielectric properties of poly(vinylidene fluoride) (PVDF) were successfully improved by incorporating with silver nanoparticles (nAg) and high-permittivity nickelate (Mg-doped La1.9Sr0.1NiO4) particles. nAg particles were directly grown on the surface of nickelate particles to produce nAg-MLSNO hybrid particles. The nAg-MLSNO/PVDF nanocomposites exhibited superior dielectric properties by filling with a very low filler loading. A composite with volume fraction f = 0.1755 exhibited an enhanced dielectric permittivity (epsilon') with retaining low conductivity (sigma approximate to 10(-8) S.m(-1)) and particularly low dielectric loss tangent (tan delta approximate to 0.027 at 1 kHz). The composite polymer matrix retained excellent flexibility because of the low concentration of fillers. Interestingly, epsilon' was slightly dependent on frequency and temperature. It can be a promising flexible dielectric polymer to fulfill needs in modern electronic applications. Low tan delta and conductivity were due to the suppressed formation of conduction path in the polymer matrix by the nAg-MLSNO hybrid particles. Significantly enhanced dielectric properties were explained based on the interfacial polarization.