Bryophytes are a group of plants that present a variety of chemical compounds, but information on the phytochemistry of the species, especially those in the Brazilian Amazon, is still scant. Thus, the objective of this work was to determine the volatile chemical constituents of the Amazonian moss species Sematophyllum subsimplex (Hedw). Mitt. and Leucobryum martianum (Hornsch.) Hampe ex Mull Hal. Samples were collected at the Gunma Ecological Park, in the municipality of Santa Bárbara, Pará, and subsequently dried, identified, screened, kept in a refrigerated place, and subjected to extraction by means of simultaneous distillation-extraction (SDE). Volatile concentrates were analyzed by gas chromatography/mass spectrometry (GC-MS). Forty-two chemical constituents were identified in the pentane extracts of the two species studied, mainly belonging to the group of aldehydes, terpenes, and carboxylic acids. Naphthalene was predominant in both species, mainly in L. martianum. Safrole, found in L. martianum, is being recorded for the first time in a moss. This study represents the first report of the chemical composition of the two selected taxa and the results indicate that these mosses are natural sources of compounds of interest for bioprospecting.