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In the current study, the PbO compound was used in order to optimize the gamma-ray shielding properties of the polypropylene polymers. A series of polypropylene doped PbO were performed using various PbO concentrations varied between 0 and 50 wt%. The experimental measurement for the density of the fabricated sample showed that the samples’ density varied between 0.902 ± 0.004 and 1.645 ± 0.007 g/cm3, raising the PbO doping concentration between 0 wt% and 50 wt%. Furthermore, the scanning electron microscope was utilized to illustrate the distribution and morphology of the fabricated polypropylene doped PbO concentrations. The gamma-ray shielding capacity of the fabricated polypropylene doped PbO was examined and evaluated experimentally using a sodium iodide scintillation detector and different point sources in the gamma-ray energy interval between 0.059 and 1.408 MeV. The experimental results were affirmed via the Geant4 code, which depended on the Monte Carlo simulation. The difference recorded between the experimental and Geant4 calculations for the fabricated samples shielding properties was lies in between ±4%. The recorded linear attenuation coefficient at gamma-ray energy of 0.244 MeV varied between 0.1148 and 0.5837 cm−1, raising the PbO doping concentration between 0 wt% and 50 wt%. Moreover, the half-value thickness decreased with increasing the PbO doping ratio.