The melt-quenching method was applied to fabricate a new glass series containing 10Bi2O3–70TeO2-(20-x)ZnO-xTa2O5, x = 0, 2, 4, and 6 mol%. The chemical compounds were well mixed and melted in a furnace at 900 °C, and then the molten transferred to another furnace at 320 °C for annealing. X-ray diffraction is used to confirm the amorphous phase of the fabricated glasses. Moreover, the fabricated glasses' structure characterization was established using Raman analyses. Besides, the gamma-ray protection capacity was evaluated for the fabricated glass series. Thus, the MCNP-5 simulation code and XCOM software program were utilized to estimate the investigated glass samples' linear attenuation coefficients. The glass sample's highest attenuation coefficient, with 6 mol % of the Ta2O5 doping ratio is ranged between 418.17 and 0.27 cm−1. In comparison, the fabricated glass without Ta2O5 possesses the lowest attenuation factor and decreased from 359.39 cm-1 to 0.26 cm−1, raising the incoming photon energy from 0.015 MeV to 15 MeV, respectively. The simulated linear attenuation coefficient was then applied to calculate the half-value thickness, and transmission factor for the incoming photons. The obtained results showed that the fabricated glass samples' shielding ability enhanced with the insertion of the Ta2O5.