BackgroundWhite tea has become more and more popular with consumers due to its health benefits and unique flavor. However, the key aroma‐active compounds of white tea during the aging process are still unclear. Thus, the key aroma‐active compounds of white tea during the aging process were investigated using gas chromatography‐time‐of‐flight‐mass spectrometry (GC‐TOF‐MS) and gas chromatography‐olfactometry (GC‐O) combined with sensory‐directed flavor analysis.ResultsA total of 127 volatile compounds were identified from white tea samples with different aging years by GC‐TOF‐MS. Fifty‐eight aroma‐active compounds were then determined by GC‐O, and 19 of them were further selected as the key aroma‐active compounds based on modified frequency (MF) and odor activity value (OAV).ConclusionAroma recombination and omission testing confirmed that 1‐octen‐3‐ol, linalool, phenethyl alcohol, geraniol, (E)‐β‐ionone, α‐ionone, hexanal, phenylacetaldehyde, nonanal, (E, Z)‐(2,6)‐nonadienal, safranal, γ‐nonalactone and 2‐amylfuran were the common key aroma‐active compounds to all samples. Cedrol, linalool oxide II and methyl salicylate were confirmed peculiar in new white tea, while β‐damascenone and jasmone were peculiar in aged white tea. This work will offer support for further studies on the material basis of flavor formation of white tea. © 2023 Society of Chemical Industry.