We aimed to investigate the aroma quality characteristics of Bai Mu Dan tea from different tea plant varieties and the material basis for quality differences among the varieties. Aroma components of Bai Mu Dan tea samples from the varieties Zhenghe Dabaicha (ZD), Fuding Dahaocha (FD), Fujian Shuixian (SX), and Meizhan (MZ) were measured using headspace solid-phase microextraction (HS-SPME) coupled with gas chromatography–mass spectrometry (GC-MS) (HS-SPME-GC-MS) and comparatively analyzed using principal component analysis (PCA), partial least squares discriminant analysis (PLS-DA), and hierarchical cluster analysis (HCA). The results indicated that all Bai Mu Dan tea varieties had excellent aroma qualities and distinct characteristics. Specifically, ZD had a fresh aroma with a floral note, FD had a delicate aroma with an obvious pekoe scent, SX had an obvious floral aroma, and MZ had a strong and lasting floral aroma. The aroma scores of the different varieties were in the order MZ>SX>FD>ZD>90 points. A total of 101 aroma components were detected in the Bai Mu Dan tea varieties, with 98, 98, 100, and 96 aroma components identified in ZD, FD, MZ, and SX, respectively. The aroma components mainly consisted of alcohols, hydrocarbons, esters, and ketones. PCA and PLS-DA models, which enabled the effective distinguishing of different Bai Mu Dan tea varieties, were constructed based on the relative contents of all aroma components. Thirteen aroma components had significantly different contents (VIP>1, p<0.05) in different Bai Mu Dan tea varieties. In conclusion, the four investigated Bai Mu Dan tea varieties exhibited significant differences in aroma quality characteristics and distinct aroma profiles, and 13 aroma components were identified as key components that contributed to quality differences among varieties.