Apart from geographical difference and processing method, the maturity of fresh tea shoot is an important factor that determines tea quality. However, the quality development and chemical variation of green tea with tea shoot maturity remain unclear. This study aimed to investigate the metabolic consequences of tea shoot maturity on the taste and aroma quality of green tea by metabolite profiling. In terms of taste quality, a concentration-dependent decrease with tea shoot age was observed in gallic acid and caffeine. The levels of catechin, epicatechin, and epigallocatechin increased with tea shoot maturity, whereas those of epicatechin gallate, epigallocatechin gallate, and total catechins decreased. Furthermore, the maximum contents of most amino acids were recorded in green tea processed from one bud with two leaves. In terms of aroma quality, volatile profiles of green tea were analyzed by gas chromatography–mass spectrometry combined with chemometrics. A total of 32 differential volatile organic compounds showing significant differences were identified and divided into Groups I and II, which contribute undesirable flavor and sweet flowery aroma to tea, respectively. The relative abundance of Group I increased with tea shoot maturity whereas that of Group II decreased. These findings can be used in guiding the production of green tea.
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