Shangri-La is a promising wine region in China, which has great potential for producing high-quality wines with distinctive regional characteristics. In this work, the aroma properties of spontaneously fermented Cabernet Sauvignon wines produced from seven sub-regions of Shangri-La (Adong, Liutongjiang, Sinong, Xidang, and Nitong from Lancang River basin; Benzilan and Dari from Jinsha River Basin) were comprehensively analyzed using the headspace micro-extraction with gas chromatography-mass spectrometry, odor activity values, and olfactory evaluation. Results showed that a total of 59 volatiles belonging to seven groups were identified and quantified in all regional wines, with alcohols constituting the most abundant group, followed by esters and volatile fatty acids. Based on their odor activity values, six alcohols, seven esters, two terpenes, one C13-norisoprenoids, and three volatile fatty acids were identified as key volatiles which significantly contribute to the aroma of these wines. Principal component analysis showed the distinct compositions of these 19 key volatiles among the seven regional wines. Olfactory evaluation revealed certain differences in aroma profiles, particularly "Tropical fruit", "Dried fruit", "Vegetal", and "Sweet" among them. This study enhances our understanding on the unique terroir flavors of Shangri-La wines and is helpful for further producing high-quality wines with regional characteristics.