Twenty‐nine compounds were identified as the key volatiles from 237 volatiles, which formed the flowery aroma of PCT. Linalool, geraniol, nonanal, and methyl salicylate were more abundant in the PCT, and they evoked the top five emotions, including mild, wild, aggressive, tame, and bored. Methyl salicylate contributed most to the wild emotion in the two mixed samples, and it may contribute positively to the health effects of tea. Abstract Pu'er crude tea (PCT), the initial raw material for making Pu'er tea, is favored because of unique flavor ...