There is a lack of theoretical evidence regarding the transformation of the aroma of Pu-erh tea (raw tea) during long-term storage. In this study, we comprehensively investigate the aroma characteristics of Pu-erh tea (raw tea) from the same manufacturer, stored for different storage times (7-21 years). Sensory evaluation and qualitative and quantitative analysis of volatile substances were performed on the experimental samples. The results showed that the aroma of Pu-erh tea (raw tea) changed from fruity/floral to smoky and fragrance during the storage process. A total of 290 volatiles were identified by HS-SPME/GC×GC-Q-TOF-MS. The key substances for the fruity/floral aroma are fenchene, (E)-1,2,3-trimethyl-4-propenyl-Naphthalene, (+/--theaspirane, and decanal, and the key substances for the smoky aroma were 2-ethyl-Furan, camphene, 1-methyl-4-(1-methylethenyl)-Benzene, and cis-