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In the present work, the optical properties and gamma-ray shielding properties of 70[xTeO2 + (1−x)B2O3] + 15Na2O + 15K2O glasses have been investigated. The optical band gap ( E o p t ) showed an initial decrease for x ≤ 10 mol% and then increased for x >10 mol%, which is suggested to be related to the changes in concentration of non-bridging oxygen (NBO). Urbach energy ( E u ) behaves inversely with E o p t . Within the same region, refractive index (n) also exhibited an off-trend pattern that signified polarizability difference led by alteration in bridging oxygen and NBO concentration. The mass attenuation coefficient (MAC) derived from interpolation of EPICS2017 in ENDF/B-VIII were in good agreement with generated values of XCOM and showed a decreasing trend with increasing gamma photon energy from 59.5 keV to 1333 keV. The linear attenuation coefficient (LAC) also showed a decreasing trend with the increase in energies from 59.5 to 1333 keV, which indicates that the prepared TeO2-B2O3-Na2O-K2O glasses can effectively shield the low energy photons, while this ability to shield the photons becomes weaker with increasing energy. The results revealed that the sample with no TeO2 has a relatively higher mean free path (MFP) compared to other samples, and the addition of TeO2 highly affects the MFP values. Thus, the glass with no TeO2 requires a much higher thickness than the remaining glasses to attenuate the photons and to provide sufficient protection from radiation.