(Tl2O3)(30)-(Li2O)(10)-(B2O3)((60-y)())-(Sm2O3)(y) glass system with various Sm2O3 additives (y = 0, 0.2, 0.4, 0.6) was studied in detail. The vibrational modes of the (Tl2O3)(30)-(Li2O)(10)-(B2O3)((60-y)) network were active at three composition-related IR spectral peaks that differed from those mixed with Samarium (III) oxide at high wavenumber ranges. These glass samples show that their permeability increased with the Samarium (III) oxide content increase. Additionally, the electronic transition between localized states was observed in the samples. The MAC, HVL, and Zeff values for radiation shielding parameters were calculated in the energy range of 0.015-15 MeV using the FLUKA algorithm. In addition, EBF, EABF, and sigma(R) values were also determined for the prepared glasses. These values indicated that the parameters for shielding (MAC, HVL, Z(eff), EBF, EABF, and sigma(R)) are dependent upon the Samarium (III) oxide content. Furthermore, the addition of Samarium (III) oxide to the examined glass samples greatly reinforced their shielding capacity against gamma photon. The findings of the current study were compared to analyses of the XCOM software, some concretes, and lead. In the experiment, it was found that the SMG0.6 glass sample was the strongest shield.