Keemun, Assam, Darjeeling and Ceylon black teas are honored as the world's four most famous black teas, and their excellent aroma qualities are well received by people around the world. In this study, aroma components in these four types of teas were analyzed by comprehensive two-dimensional gas chromatography time-of-flight mass spectrometry (GC × GC-TOFMS) and gas chromatography-olfactometry (GC-O) technologies. A total of 42 aroma-active compounds were ultimately identified, especially benzeneacetaldehyde, geraniol, (Z)-3-hexen-1-yl hexanoate, trans-β-ionone, cis-linalool oxide (pyranoid), hotrienol, and methyl salicylate presented the strongest aroma strengths with pleasant scents in all tested teas. The quantification results indicated that 19 compounds including (Z)-3-hexenol, 1-octen-3-ol, linalool, phenylethyl alcohol, hexanal, benzeneacetaldehyde, limonene, heptanoic acid, (Z)-3-hexen-1-ol, acetate, benzyl alcohol, trans-linalool oxide (furanoid), hotrienol, 1-octen-3-one, 2-nonanone, (E)-2-octenal, nonanal, β-myrcene, 2-pentylfuran, and methylpyrazine were identified as the key compounds with odor activity values (OAVs) higher than 1.0 in the world's four most famous black teas. Notably, the comparison of GC-O and OAV calculation results showed that methyl salicylate (Ceylon), (E)-2-octenal (Assam), benzeneacetaldehyde (Keemun) and linalool and trans-linalool oxide (furanoid) (Darjeeling) might be the most definitive odorants in the corresponding tea categories.