Lapsang Souchong black tea enjoys a good reputation in China for its unique smoky flavor. A total of 61 odorants in smoked Lapsang Souchong (SLS) and 49 odorants in the reference sample (non-smoked Lapsang Souchong, NSLS) were identified, respectively. The odorants of tea origin decreased significantly after the smoking process, while the pyrolysis products of pine wood increased markedly. Phenols (66.6%) were the most abundant odorants in SLS, among them, 18 phenols were newly found compared to NSLS. Aroma recombinates of SLS and NSLS proved the successful identification and quantitation of their respective key aroma compounds. The omission and addition tests clearly corroborated 3-ethylphenol, p-cresol, m-cresol, and 2-methoxy-4-methylphenol were the crucial factor for the strong smoky pine aroma characteristics of SLS tea. The findings offer a new insight into the flavor role of phenols to SLS tea, which will help to deeply explore the effect of smoking process on aroma changes during tea production.