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Based on lithium aluminosilicate glass, the composition of glass was optimized by replacing SiO₂ with B₂O₃, and the influence of glass composition on structure and performance was studied. With the increase in B₂O₃ concentrations from 0 to 6.5 mol%, Al₂O₃ always existed in the form of four-coordinated [AlO₄] in the network structure, and B₂O₃ mainly entered the network in the form of four-coordinated [BO₄]. The content of Si-O-Si linkages (Q₄^(0Al)) was always dominant. The incorporation of boron oxide improved the overall degree of polymerization and connectivity of the lithium aluminosilicate glass network structure. An increase in the degree of network polymerization led to a decrease in the thermal expansion coefficient of the glass and an increase in Vickers hardness and density. The durability of the glass in hydrofluoric acid and NaOH and KOH solutions was enhanced overall.