The present study sought to characterize the composition of volatile aroma compounds and key aroma-active compounds of dried Hanyuan Zanthoxylum bungeanum. The volatile aroma compounds were analyzed by the solid-phase microextraction (SPME) combined with gas chromatography-olfactometry-mass spectrometry (GC-O-MS) and two-dimensional comprehensive gas chromatography-olfactometry-mass spectrometry (GC x GC-O-MS). The key aroma-active compounds were analyzed by the aroma extract dilution analysis and odor activity value. A total of 72 volatile compounds were identified by GC-O-MS, of which 28 were aroma-active. Meanwhile, 116 volatile compounds were identified by GC x GC-O-MS, of which 43 were aroma-active. These results revealed that myrcene, (+)-limonene, (E)-beta-ocimene, beta-cubebene, Germacrene D, cineole, linalool, and linalyl acetate were the key aroma-active compounds of dried Hanyuan Zanthoxylum bungeanum.