Penthorum chinense Pursh (Penthoraceae) is a traditional herb used in Miao medical systems that is also processed into foods (e.g., tea products) in China. Different processing methods significantly affect the volatile compounds, phenolic constituents, and biological activities. This study aimed to produce P. chinense green tea leaves (GTL), black tea leaves (BTL), and untreated leaves (UL) to investigate differences in their flavor substances, functional components, antioxidant activity, alcohol dehydrogenase (ADH) activity, and acetaldehyde dehydrogenase (ALDH) activity. The results showed that 63, 56, and 56 volatile compounds were detected in UL, GTL, and BTL, respectively, of which 43 volatile compounds were identified as differential metabolites among them. The total phenolic content (97.13–179.34 mg GAE/g DW), flavonoid content (40.07–71.93 mg RE/g DW), and proanthocyanidin content (54.13–65.91 mg CE/g DW) exhibited similar trends, decreasing in the order of UL > BTL > GTL. Fourteen phenolic compounds were determined, of which gallic acid, (−)-epicatechin, and pinocembrin 7-O-glucoside showed a sharp decrease in content from UL to BTL, while the content of pinocembrin 7-O-(3″-O-galloy-4″, 6″-hexahydroxydiphenoyl)-glucoside and pinocembrin significantly increased. GTL showed better DPPH/ABTS·+ scavenging ability and ferric-reducing ability than UL. The ADH and ALDH activities decreased in the order of GTL > UL > BTL. Therefore, tea products made with P. chinense leaves contained an abundance of functional compounds and showed satisfactory antioxidant and hepatoprotective activities, which are recommended for daily consumption.
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