Development of polymers with excellent dielectric properties is a challenge for advanced electronic devices. Impregnating conducting fillers like carbon nanoparticles can enhance the dielectric constant, retaining low loss due to its compatibility and favorable polarization within the polymer matrix. The multifunctional characteristics of coal-derived nanocarbon can improve permittivity and facilitate large-scale production at a lower cost. The incorporation of coal-based nanocarbon in the polymer matrix and its dielectric response is seldom investigated. In this work, different ratios (10:90, 50:50, 90:10 by weight) of nanocarbon/PVDF composite are prepared via a simple solution casting technique. The dielectric measurements show that nanofillers’ addition significantly augments the dielectric constant value, which is ∼3 times (50:50 composite) higher than pure PVDF. The uniform distribution of 50% filler within the polymer matrix impeded the seepage of charge at the interface and enhanced the permittivity via polarization of accumulated charges. The composite also exhibited balanced dielectric loss that is essential for energy storage applications.