Aroma is an indispensable factor that substantially impacts the quality assessment of black tea. This study aims to uncover the dynamic alterations in the sweet and floral aroma black tea (SFABT) throughout various manufacturing stages using a comprehensive analytical approach integrating gas chromatography electronic nose, gas chromatography–ion mobility spectrometry (GC-IMS), and gas chromatography–mass spectrometry (GC-MS). Notable alterations in volatile components were discerned during processing, predominantly during the rolling stage. A total of 59 typical volatile compounds were identified through GC-IMS, whereas 106 volatile components were recognized via GC-MS throughout the entire manufacturing process. Among them, 14 volatile compounds, such as linalool, β-ionone, dimethyl sulfide, and 1-octen-3-ol, stood out as characteristic components responsible for SFABT with relative odor activity values exceeding one. This study serves as an invaluable theoretical platform for strategic controllable processing of superior-quality black tea.

Aroma plays a pivotal role in the quality of black tea. However, the acceptability of black tea is greatly limited by the green off-flavor (GOF) resulting from the inappropriate processing control. In this study, the key odorants causing GOF were investigated by volatolomics, and their dynamic changes and formation pathways were in-depth understood. Significant alterations in volatile metabolites were observed in the withering stage. A total of 14 key odorants were identified as contributors to GOF, including 2-methylpropanal, 3-methylbutanal, 1-hexanol, nonanal, (E, E)-2,4-heptadienal, benzaldehyde, linalool, (E, E)-3,5-octadiene-2-one, β-cyclocitral, phenylacetaldehyde, (E, E)-2,4-nonadienal, methyl salicylate, geraniol, and β-ionone. Among them, (E, E)-2,4-heptadienal (OAV = 3913), characterized by fatty, green, and oily aromas, was considered to be the most important contributor causing GOF. Moreover, it was found that lipid degradation served as the primary metabolic pathway for GOF. This study provides a theoretical foundation for off-flavor control and quality improvement of black tea.