Ripened pu-erh tea is a post-fermented tea produced from sun-dried green tea in the Yunnan province of China. The headspace-solid phase microextraction-gas chromatography-tandem mass spectrometry (HS-SPME/GC-MS) technique was used to analyze the changes in the relative content of aroma constituents of two ripened pu-erh tea sample groups with different sensory scores for aroma quality. Correlation analysis and principal component analysis showed that the relative levels of 3,4,5-trimethoxy-benzaldehyde, dimethyl itaconate, butanoic acid-2-ethyl-2-propenyl ester, 3,4-dimethoxytoluene, 1,2,3-trimethoxy-5-methyl-benzene, and other aroma constituents showed a significant correlation with the aroma quality score obtained from the sensory evaluation（p < 0.01). The relative content of nerol, nerolidol, and n-hexadecanoic acid were significantly correlated with the aroma the quality score (p < 0.05). This result suggests that the above-mentioned compounds are the key aroma constituents influencing the aroma quality of ripened pu-erh tea. Moreover, a preliminarily partial least squares (PLS) regression model was constructed based on the levels of these key aroma compounds to predict the aroma quality of ripened pu-erh tea.