A new flavone glycoside, 6-hydroxyluteolin 7-O-[6 '''-benzoyl-beta-D-glucopyranosyl-(1 -> 2)]-beta-D-glucopyranoside (aphyllanthoside, 1) was isolated from the MeOH extract of the aerial parts of Globularia aphyllanthes. Besides this new compound, two flavonoid glycosides (6-hydroxyluteolin 7-O-[6 '''-(E)-caffeoyl-beta-D-glucopyranosyl-(1 -> 2)]-beta-D-glucopyranoside and isoquercitrin), three phenylethanoid glycosides (verbascoside, rossicaside A, and trichosanthoside A), and 11 iridoid glycosides (aucubin, catalpol, 10-O-benzoylcatalpol, globularin, asperuloside, besperuloside, asperulosidic acid, daphylloside, scandoside, alpinoside and baldaccioside) were also obtained and characterized. Identification of the isolated Compounds was carried out by spectroscopic analysis including I D and 2D NMR experiments as well as HRMS.