Cobalt-doped titania nanocomposites were fabricated to be utilized for radiation shielding aims. The chemical composition of the composites was measured using the energy-dispersive X-ray spectrometer. Moreover, the structure of the composites was evaluated using the X-ray diffractometer, and the morphology of the fabricated composites was presented using the scanning electron microscope. Furthermore, the γ-ray shielding properties were estimated using the Monte Carlo simulation between 0.059 and 2.506 MeV. The linear attenuation coefficient of the fabricated composites decreased by factors of 93% for all samples by raising the incident γ-energy between 0.059 and 2.506 MeV. Moreover, the partial replacement of the Ti4+ by Co3+ slightly enhanced the linear attenuation coefficient from 0.607 to 0.630 cm−1 when the Co3+ increased from 0 to 3.7 wt%. The improvement in the linear attenuation coefficient causes an enhancement in other radiation shielding properties.