The Chinese yam ( Dioscorea opposita) is a basic food in Asia and especially China. Consequently, an uncomplicated, reliable method should be available for the analysis of the quality and origin of the yams. Thus, near-infrared (NIR) and mid-infrared (mid-IR) spectroscopic methods were developed to discriminate among Chinese yam samples collected from four geographical regions. The yam samples were analyzed also for total sugar, polysaccharides, and flavonoids. These three analytes were used to compare the performance of the analytical methods. Overlapping spectra were resolved using chemometrics methods. Such spectra were compared qualitatively using principal component analysis (PCA) and quantitatively using partial least squares (PLS) and least squares-support vector machine (LS-SVM) models. We discriminated among the four sets of yam data using PCA, and the NIR data performed somewhat better than the mid-IR data. We constructed the PLS and LS-SVM calibration models for the prediction of the three key variables, and the LS-SVM model produced better results. Also, the NIR prediction model produced better outcomes than the mid-IR prediction model. Thus, both infrared (IR) techniques performed well for the analysis of the three key analytes, and the samples were qualitatively discriminated according to their provinces of origin. Both techniques may be recommended for the analysis of Chinese yams, although the NIR technique would be preferred.