Changes in key odorants of shaken black tea (SBT) during its manufacture were determined using headspace solid-phase microextraction (HS-SPME) combined with comprehensive two-dimensional gas chromatography–time-of-flight mass spectrometry (GC × GC–TOFMS) and multivariate data analysis. A total of 241 volatiles was identified, comprising 49 aldehydes, 40 esters, 29 alcohols, 34 ketones, 30 aromatics, 24 alkenes, 17 alkanes, 13 furans, and 5 other compounds. A total of 27 volatiles had average relative odor activity values (rOAVs) greater than 1, among which (E)-β-ionone, (E,Z)-2,6-nonadienal, and 1-octen-3-one exhibited the highest values. According to the criteria of variable importance in projection (VIP) > 1, p < 0.05, and |log₂FC| > 1, 61 discriminatory volatile compounds were screened out, of which 26 substances were shared in the shaking stage (FL vs. S1, S1 vs. S2, S2 vs. S3). The results of the orthogonal partial least squares discriminate analysis (OPLS-DA) differentiated the influence of shaking, fermentation, and drying processes on the formation of volatile compounds in SBT. In particular, (Z)-3-hexenol, (Z)-hexanoic acid, 3-hexenyl ester, (E)-β-farnesene, and indole mainly formed in the shaking stage, which promoted the formation of the floral and fruity flavor of black tea. This study enriches the basic theory of black tea flavor quality and provide the theoretical basis for the further development of aroma quality control.

Phenolic acids are important taste components in green tea. The aim of this study was to analyze the taste characteristics of phenolic acids and their influence on the bitterness and astringency of green tea by sensory evaluation and chemical determination. The major tea phenolic acids and quercetin-3-O-rutinoside (Que-rut) were significantly positively correlated with the bitterness (r = 0.757, p < 0.01; r = 0.605, p < 0.05) and astringency (r = 0.870, p < 0.01; r = 0.576, p < 0.05) of green tea infusion. The phenolic acids have a sour and astringent taste, whereas Que-rut has a mild astringent taste. Phenolic acids and Que-rut can increase the bitterness of epigallocatechin gallate (EGCG). However, these components behaved differently for astringency on EGCG. Gallic acid (GA) enhances the astringency throughout all the concentrations in this study. While it seemed to be double effects of caffeic acid (CA), chlorogenic acid (CGA), and Que-rut on that, i.e., the inhibition at lower concentrations (CA: 0–0.2 mM; CGA: 0–0.2 mM; Que-rut: 0–0.05 mM) but enhancement at higher ones. The phenolic acids and Que-rut interacted synergistically with tea infusion and as their concentration increased, the synergistic enhancement of the bitterness and astringency of tea infusion increased. These findings help provide a theoretical basis for improving the taste of middle and green tea.