In order to investigate the differences in the characteristic aroma of black teas from different regions, the volatile aroma compounds of Keemun black tea, Yichang black tea, Dianhong black tea and Yingde black tea were identified by solid phase extraction (SPE) combined with gas chromatography-mass spectrometry (GC-MS) and were evaluated by gas chromatography-olfactory (GC-O). Odor activity value (OAV) calculation and correlation analysis between sensory aroma profile and key aroma-active compounds were performed to analyze the sensory attributes and chemical basis of the characteristic aroma of black tea. The results showed that the four black teas differed in the sensory attributes of seven aroma notes such as floral, sweet and herbal notes. Additionally, 24 differential key aroma compounds were identified (P < 0.05, OAV > 1). Geraniol contributed most to black tea aroma with the highest OAV in Keemun black tea (16581.33), followed by Yichang black tea (7463.65), Dianhong black tea (2832.13) and Yingde black tea (467.96). Partial least squares (PLS) regression analysis and Pearson correlation analysis showed that β-ionone, geraniol and indole were responsible for the floral and sweet aroma of Keemun black tea, (Z)-3-hexenol and α-terpineol contributed to the fruity and woody aroma of Dianhong black tea, and 2-heptanol and (Z)-linalooloxide were responsible for the herbal aroma of Yingde black tea. In conclusion, this study has preliminarily clarified the characteristic aroma profiles of black tea from the four regions and their material basis at the molecular level.