The research on development of nanodielectric material is the requirement of capacitor industry. The polymeric material could not have a high dielectric constant due to limitation of structure and physical properties. However, combination of suitable nanofiller can increase the dielectric constant several times. We have reported the dielectric properties of polysulfone + ZnO nanodielectric system. The dielectric properties are observed to be governed by dipolar polarization fully and interfacial polarization partially. The relaxation time of dipoles is quite high: It means that nanodipoles have sufficient relaxation time to orient in the direction of field. Interface provides additional trapping level for storage of charge carriers energetically. The permittivity of new material increases many times of base material even at lower concentration of fillers.