This study focuses on enhancing the attenuation properties of bentonite clay using powdered iron and ferrosilicon. Scanning electron microscopy and X-ray diffraction analysis were used to characterize the prepared samples. The linear attenuation coefficient was calculated experimentally for the prepared samples using a NaI scintillation detector and four radioactive point sources (Am-241, Cs-137, Co-60, and Eu-152). These results were in good agreement with the compared with the XCOM results. Other radiation shielding parameters, such as the half-value layer, mean free path, and radiation protection efficiency, were determined. Furthermore, at a photon energy of 0.06 MeV, the half-value layers were 0.276 and 0.628 cm for bentonite–iron and bentonite–ferrosilicon, respectively. The results indicate that the radiation shielding efficiency of bentonite–iron composites is better than that of bentonite–ferrosilicon composites at low and intermediate gamma-ray energies.