Fruiting bodies and mycelia of Grifola frondosa were produced by solid-state and submerged cultures, respectively. The volatile compounds of fruiting bodies and mycelia were analyzed by headspace solid-phase microextraction (HS-SPME) combined with gas chromatography-mass spectrometry (GC-MS). The results showed that fruiting bodies and mycelia of Grifola frondosa, respectively, contained 62 and 94 volatile compounds. Hereinto, 37 compounds in both fruiting bodies and mycelia accounted for 86.81% and 84.28% of total volatile substances, respectively. The fruiting bodies mainly contained alcohol (14), ketones (13), formaldehyde (12), acid (7), esters (5), and so on. Esters (42.80%) and aldehydes (35.14%) were the main volatile compounds of fruiting bodies, and the relative content of ethyl acetate was 42.57%. The mycelia mainly contained formaldehyde (22), ketones (17), alcohol (16), esters (13), acid (12) and so on, of which aldehydes, esters, acids and alcohols, respectively, accounted for 47.0%, 10.90%, 7.48% and 5.94%. The content of isovaleraldehyde and lichen phenol reached 23.31% and 15.41%, respectively.