Abstract Four different extraction methods were used to extract aroma compounds from flour. It was found that dynamic headspace sampling (DHS) was a better method for extracting aroma-active compounds in flour. Hexanal, decanal, butanoic acid, 2,3-pentanedione, 2-acetyl-1-pyrrolinoline, and 3-octen-2-one were found to be the important aroma-active compounds in flour by olfaction (O) in two-dimensional gas chromatography–olfactometry–mass spectrometry (GC×GC-O-MS). Dynamic headspace dilution analysis (DHDA), odour activity value (OAV), recombination and omission experiment further verified that these compounds can roughly simulate the overall aroma profile of flour. In this study, we determined the aroma-active compounds in flour by molecular sensory science to improve the sensory preference of flour and enhance the quality of flour aroma, which will provide analytical ideas for future research on flour aroma and improve the production process.