Visible/near infrared spectroscopy (Vis/NIRs) technique was applied to non-destructive quantification of sugar and pH value in yogurt. Partial least squares (PLS) analysis and least squares support vector machine (LS-SVM) were implemented for calibration models. In this paper, three brands (Mengniu, Junyao, and Guangming) were set as the calibration, and the remaining two brands (Yili and Shuangfeng) were used as prediction set. In the LS-SVM model, the correlation coefficient (r), root mean square error of prediction, and bias in prediction set were 0.9427, 0.2621°Brix, 1.804e−09 for soluble solids content, and 0.9208, 0.0327, and 1.094e−09 for pH, respectively. The correlation spectra corresponding to the soluble solids content and pH value of yogurt were also analyzed through PLS method. LS-SVM model was better than PLS models for the measurements of soluble solids content and pH value. The results showed that the Vis/NIRs combined with LS-SVM models could predict the soluble solids content and pH value of yogurt.