The volatile compounds of tartary buckwheat extract was extracted by solidphase micro-extraction (SPME) and analyzed by gas chromatography-mass spectrometry (GC-MS). Then aroma-active compounds were identified by gas chromatography-olfactory (GC-O) combined with aroma extraction dilution analysis (AEDA). Finally, the key odorants of tartary buckwheat extract were confirmed by their odor activity values (OAVs). The results showed that 92 kinds of volatile compounds including 28 esters, 7 aldehydes, 9 alcohols, 7 ketones, 6 acids, 8 olefins, 20 alkanes, and 7 others were identified by SPME-GC-MS. By application of GC-O/AEDA, seventeen odor-active compounds with flavor dilution (FD) factor range from 1 to 243 were detected. Quantitation results showed that benzyl alcohol (8637.43 μg/kg), phenylacetaldehyde (3150.47 μg/kg), and D-limonene (3080 μg/kg) had a higher concentration. Finally, benzaldehyde, dimethyl trisulfide, benzyl alcohol, phenylacetaldehyde, diethyl malonate were confirmed as the key odorants of the tartary Buckwheat extract for their highest FD factors and OAVs.