In this research, we present a novel methodology for the production of Pb(ZrO3)-doped zirconia derived from zircon minerals. Our approach involves the fabrication of two composite samples via a streamlined hydrothermal synthesis process, offering a direct pathway to manufacture. Furthermore, we conducted an extensive analysis of the recently synthesized compounds using advanced techniques such as X-ray diffraction, scanning electron microscopy, and transmission electron microscopy. Additionally, we investigated the average size of crystallites in the prepared samples and examined their correlation with lattice distortions and dislocation density. Additionally, the Monte Carlo simulation code examined the γ-ray shielding properties of the fabricated lead-based zirconate ceramic composites. The evaluation shows an enhancement in the linear attenuation coefficient of the fabricated composites from 0.411 to 0.464 cm−1 (at γ-ray energy of 0.662 MeV), raising the Pb concentration from 6.6 to 13.3 wt%. The enhancement in the linear attenuation coefficient decreases the lead equivalent thickness of the fabricated composites where the thickness of composites equivalent to 1 cm of pure lead is reduced to 2.68 cm by raising the Pb concentration to 13.3 wt%. The shielding evaluation for the fabricated composites showed a high performance against low and intermediate γ-ray photons where the shielding capacity of the fabricated composites reaches 37% and 47% of the pure lead shielding capacity at γ-ray energy of 0.662 MeV and 2.506 MeV, respectively. Therefore, the fabricated composites can be used as an alternative shielding material in hospitals and radioactive zones.