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IR Li2Ga2GeS6 nonlinear crystals were directly obtained with the composition of 40GeS2-30Ga2S3-30Li2S, by the conventional melt-quenching method. The high depth digital image indicated that the obtained Li2Ga2GeS6 crystals showed a big size of 0.3 × 0.25 × 0.3 mm3. It was shown that the compound was very susceptive to H2O with second harmonic observation. Besides, the glass-forming region of GeS2-Ga2S3-Li2S system was further studied by the conventional melt-quenching method.GeS2-Ga2S3-Li2S glass-ceramics containing IR Li2Ga2GeS6 nonlinear nanocrystals were obtained at a more carefully controlled heating rate.