This work aims to prepare a new series of polyepoxide resins reinforced with a mixture of WO3 and Bi2O3 compounds. The effect of replacing WO3 with by Bi2O3 on the radiation shielding parameters was experimentally evaluated using a NaI (Tl) detector and many radioactive sources, including 22Na, 133Ba, 137Cs, 60Co, and 152Eu. The linear attenuation coefficient for the prepared new polyepoxide-based composites was improved when substituting increasing amounts of WO3 with Bi2O3. When increased from 2.164 to 2.943 cm−1 (at 33 keV) and from 0.073 to 0.104 cm−1 (at 1332 keV), the Bi2O3 concentration in the prepared composites varied from 0 to 10 wt%, respectively. The substitution of WO3 with Bi2O3 greatly improved the shielding parameters of the fabricated composites. The half-value thickness, transmission factor, and lead-equivalent thickness were observed to decrease with increasing concentrations of Bi2O3 in the fabricated composites.