By the substitution of Al 2 O 3 and B 2 O 3 for SiO 2 of the glass network former, the structural and thermal, visco-elastic and physical properties of aluminosilicate glass were investigated. 27 Al NMR results showed that in the glass structure of the system, Al 3+ basically existed in the form of 4-coordinated [AlO 4 ] tetrahedron as the network former. Judged by Raman spectra, the bridging vibration Si-O b increased with the Al 2 O 3 /SiO 2 substitute. And the total non-bridging vibration Si-O nb decreased, indicating the enhancement of the structure compactness. While for B 2 O 3 /SiO 2 substitute, the vibration at around 1010 cm −1 and the bridging vibration Si-O b in Q 4 unit both decreased and the structure got loosened. Based on the study of the structure of glass, the thermal, viscoelastic, and physical properties such as viscosity, coefficient of the linear thermal expansion, high-temperature resistance, strain point, annealing point, and softening point, aswell as density and elastic modulus were investigated. The evaluation of the melting and fining process was also investigated by high-temperature observation test. Furthermore, the chemical strengthening properties of glass samples were also investigated. The introduction of B 2 O 3 benefited for the ion-exchange. In this study, the glass composition of sample 4 was suitable for the floating process under comprehensive consideration.