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Germanate laser glasses have received much attention as a promising host materials for mid‐infrared fiber lasers in recent years because of the outstanding infrared transparency, low phonon energy, and high rare earth solubility of such glasses. However, the development of high‐performance germanate laser glasses is usually based on intuition and a trial‐and‐error method, which can involve long experimental periods and high costs, and thus, this approach is highly inefficient. Recently, with proposals for materials genome engineering, the concept of the “glass genome” has grown of interest to us. Herein, the structures of Tm3+‐doped germanate laser glasses (BaO–GeO2 and BaO–La2O3–GeO2) were investigated by Fourier transform infrared spectra (FTIR) and Raman spectra analyses, which revealed that the resulting glass contains similar structural groups to the neighboring congruently melted glassy compounds (NCMGCs) in the composition diagram. What is more, the structure and properties of the resulting laser glasses largely depend on NCMGCs. Then, the glass‐forming region, physical properties, and luminescence properties were calculated via the use of NCMGCs in Tm3+‐doped BaO–GeO2 binary and BaO–La2O3–GeO2 ternary laser glass systems. The calculated results were in good agreement with the experimental results, thus demonstrating that our approach is practical for predicting the glass‐forming region, physical properties, and luminescence properties in Tm3+‐doped BaO–GeO2 binary and BaO–La2O3–GeO2 ternary laser glass systems. This work may provide an effective method to develop Tm3+‐doped germanate laser glasses rapidly and at low cost.

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