The present investigation deals with the effects of the (gamma) γ-radiation and samples’ aging on the ac electrical properties of ultrafine iron polystyrene composites. The composites with an average thickness of 1.07 mm contain different iron particle concentrations (10, 20 and 30) by weight %. The results show that the ac electrical properties of the γ-irradiated composites are different from the non-irradiated ones. Rather relative changes in values after irradiation were registered for the impedance, dielectric constant, and the ac electrical conductivity. After irradiation, both the conductivity and the dielectric constant are enhanced relatively with the impedance becoming relatively lower in value. Also, the results show that the age of the samples affects the ac electrical properties of the tested composites. It has been found that after a few years, the electrical conductivity of the composites becomes lower in value compared to what it was a few years ago, which indicates that composites tend to lose their desired electrical properties with passage of time. So, as a potential solution for this physical behavior, the samples were exposed to γ-radiation in an attempt to enhance the metal–polymer bonding and release more free electrons within the composites. The properties such as impedance, dielectric constant, electrical conductivity of the composites were studied before and after γ-irradiation. Later, these studied electrical properties were compared with results reported few years ago. The frequency range applied in this study is consistent with Jonscher’s power law model.