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For five Ga2O3-Bi2O3-B2O3 composition glasses for improved Bi2O3 content at 25 to 65 mol% (10% continuously each time) at a fixed 10 mol% Ga2O3 amount, distinct physical and mechanical aspects and nuclear radiation attenuation factors were investigated. Increased Λ (optical basicity) values with a gradual Bi2O3 addition indicate studied samples’ improving basic character. Applying BC (bond compression) model key mechanical traits such as Ybc (Young’s modulus), Kbc (bulk modulus), S (shear modulus), L (longitudinal modulus), and σ (Poisson’s ratio) are evaluated where in all glasses 10Ga2O3-65Bi2O3-25B2O3 (mol%) sample exhibits superior elastic moduli. Enhanced Bi2O3 causes for compactness of the gallium borate network as ǹc (average cross-link density) improves from 2.3 to 3.4 indicating increased rigidity of glasses. Later, PHITS, FLUKA, and MCNPX codes are wielded to derive μ/ρ (mass attenuation coefficient) of all selected samples for photons having energy ranging from 15 KeV to 15 MeV. Simulated μ/ρ quantities exactitude is tested via Phy-X/PSD and WinXCOM programs’ μ/ρ results and identified a fairly good harmony among them. With photon energy, MFP (mean free path), TVL (tenth-value layer), and HVL (half-value layer) values variations show a similar tendency and against the trend which noticed for μ/ρ and μ (linear attenuation coefficient) values. 10Ga2O3-65Bi2O3-25B2O3 (mol%) sample’s MFP and HVL are correlated with five commercial γ-ray glass shields’ respective values at 1.25 MeV, 0.662 MeV (137Cs), and 0.2 MeV energies. Further, Zeq (equivalent atomic number) and using G–P (geometric progression) fitting approach for ten individual PDs (penetration depths) within 1–40 mfp range at 15 – 15 × 103 KeV energy region BUFs (buildup factors) were estimated. Attained RPE (radiation protection efficiency) findings attest all chosen Ga2O3-Bi2O3-B2O3 glasses’ competent absorption capacity for lower energy photons. Next, α-particles and protons MSPs (mass stopping powers), i.e. ΨA and ΨP and PRs (projected ranges), i.e. ΦA and ΦP by utilizing SRIM code as well as for electrons MSPs (ΨE) and CSDA (continuous slowing‐down approximation) ranges by ESTAR database have been calculated within 15–15 × 103 KeV KE (kinetic energy) range. Also, ΣR (fast neutron removal cross-section) and for 0.253 × 10–4 KeV energy neutrons σT (total cross-section) and SP (shielding percentage) values were approximated. With Bi2O3 addition, realized ΣR is changed at 0.1161–0.1213 cm−1 extent. For thermal neutrons absorption, 10Ga2O3-25Bi2O3-65B2O3 (mol%) glass shows larger σT (=17.534 cm−1) and at any considered thickness higher SP whereas 10Ga2O3-65Bi2O3-25B2O3 (mol%) (lead-free) glass has better attenuating features for photons affirming the incorporated Bi2O3 favorable effect.