Nine iridoid glycoside derivatives were elucidated from the methanolic extract of the aerial parts of Galium spurium (Rubiaceae) through repeated column chromatography. Their chemical structures were characterized as 10-O-trans-p-coumaroylscandoside (1a), 10-O-cis-p-coumaroylscandoside (1b), 10-O-trans-p-coumaroyl-10-O-deacetyldaphylloside (2), 10-O-cis-p-coumaroyl-10-O-deacetyldaphylloside (3), asperulic acid methylester (4), asperuloside (5), asperulosidic acid (6), scandoside (7), and deacetyl asperulosidic acid (8) by spectroscopic analysis. This is the first report of the characterization of compounds 1a, 1b, 2, 3 and 7 from this plant.