A chemical investigation of Tongoloa silaifolia led to the isolation of 12 compounds including seven coumarins, isoimperatorin (2), 7,8-dihydroxycoumarin (4), bergapten (6), phellopterin (7), isopimpinellin (8), 7-O-β-d-glucoside-8-hydroxycoumarin (11), 8-O-β-d-glucoside-7-hydroxycoumarin, (12), three flavonoids, luteolin (3), apigenin (5), luteolin-7-O-β-glucopyranoside (9), and two sterols, sitosterol (1), daucosterol (10). All of the compounds were found for the first time in Tongoloa species, while compounds 4 and 11 were new for the family Umbelliferae. The results support that coumarins are among the most characteristic and distinguishable chemical markers of the genus Tongoloa as well as of the Umbelliferae.