Abstract: To investigate the characteristic flavor profiles of Cascara Tea produced via different initial processing methods, the volatile compounds of three primary-processed samples were analyzed using gas chromatography–ion mobility spectrometry (GC-IMS) and headspace solid-phase microextraction coupled with gas chromatography–mass spectrometry (HS-SPME-GC-MS). The relative odor activity value (ROAV), in combination with chemometric analyses, was employed to evaluate differences in flavor quality among the samples. The results showed that a total of 104 volatile organic compounds (VOCs) were identified in the three Cascara Tea samples using GC-IMS, mainly including alcohols, ketones, esters, and aldehydes. Using HS-SPME-GC-MS, a total of 55 volatile organic compounds (VOCs) were identified. Specifically, 45 VOCs were detected in the dry processing sample (CX), 48 in the honey processing sample (FY), and 48 in the wet processing sample (GT). Ketones and aldehydes were the predominant aroma compounds, followed by alcohols and esters. Principal component analysis (PCA) and partial least squares-discriminant analysis (PLS-DA) revealed that the three Cascara Tea samples produced by different primary processing methods exhibited distinct differences in their compositions and concentrations of volatile compounds. The flavor profile of the CX sample was primarily associated with methyl propanoate, 2-butanone, 2,3-dihydro-3,5-dihydroxy-6-methyl-4H-pyran-4-one and 2,4-dihydroxy-2,5-dimethyl-3(2H)-furan-3-one. In contrast, the FY sample showed strong correlations with compounds such as (E)-2-decenal, butyl propanoate, furfural and 5-(acetoxymethyl)-2-furaldehyde. Meanwhile, GT sample was most strongly correlated with hexyl acetate, 2-octanone, geranyl acetone and dodecanoic acid. Based on the variable importance in projection (VIP) values from the PLS-DA model and the relative odor activity value (ROAV), seven key aroma markers were identified: (E)-2-decenal, 1-hexanol, 3-methylbutanal, butyl acetate, ethyl heptanoate, 2-furfurylthiol and 2, 4-dihydroxy-2, 5-dimethyl-3(2H)-furan-3-one. Aroma profile analysis indicated that the aroma characteristics of Cascara Tea varied among different primary processing methods. The GT sample was characterized by more pronounced acidic, spicy, nutty, and roasted notes, whereas the FY sample displayed a distinctive floral aroma. The CX sample, on the other hand, exhibited stronger nutty and roasted characteristics. This study provides a scientific reference for raw material selection and evaluation and optimization of the flavor quality of Cascara Tea during primary processing.