CuGaS2 quantum dots glass has been synthesized by both sol-gel and atmosphere control methods in this paper.The microstructures of CuGaS2 quantum dots in the glass was characterized by means of X-ray powder diffraction (XRD),X-ray photoelectron spectroscopy (XPS), transmission electron microscopy (TEM),energy dispersion X-ray spectra (EDX), high-resolution transmission electron microscopy (HRTEM), and selected-area electron diffraction (SAED).Meanwhile,the third-order nonlinear optical properties of the glass were measured in detail by the femtosecond Z-scan technique at a wavelength of 800 nm.The results showed that CuGaS2 quantum dots had been formed in the glass, and the average size of CuGaS2 quantum dots was about 12.8 nm, moreover, the glass exhibited the excellent third-order nonlinear optical properties, and the third-order nonlinear optical refractive index γ, absorption coefficient β and susceptibility x(3) of the glass were determined to be 1.57×10-9 m2/W, 2.69×10-9 m/W, and 2.24×10-17 m2/W2, respectively.