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In order to study the aroma-active components of pungent spices and to promote the standardization of their processing and application, this work used solvent-assisted flavor evaporation (SAFE) combined with gas chromatography-mass spectrometry/olfactometry (GC-MS/O) to qualitatively and quantitatively analyze the aroma-active components of 20 pungent spices. Using olfactory analysis, a total of 203 aroma-active compounds with flavor dilution (FD) values ≥ 9 were identified mainly consisting of alcohols, sulfur compounds, olefins, esters, ketones, aldehydes, phenols and acids, and the concentrations of aroma-active compounds varied between different spices. Principal component analysis (PCA) showed that all samples could be well classified into three groups. The aroma-active compounds of garlic, Welsh onion, chive and onion were dominated by sulfur compounds, while the aroma-active components of the other pungent spices were dominated by olefins, alcohols, phenols and ketones. Aroma-active sulfur-containing compounds were detected in garlic at the highest level of 3 484 777.68 μg/kg, including disulphide and trisulphide, contributing to the characteristic flavor of Allium plants. The highest content of aroma-active olefinic compounds of 72 847 224.14 μg/kg was detected in ginger, and the major aroma-active components of ginger were α-gingerene and β-sesquiterpene. Alcohols and ketones were detected in wild mint at high levels of 284 886.09 and 196 167.66 μg/kg, respectively, and the characteristic aroma components of wild mint were menthol and carvone. Aroma-active aldehydes were detected in litsea at high levels of 469 242.68 μg/kg. The major aroma-active components detected in litsea were citral and citronellal. This study provides a theoretical basis for the deep processing of pungent spices.