The aerial parts of Centaurea calcitrapa yielded cnicin, cnicin 4′-acetate, melitensin, a related elemanolide, the two new germacranolides 11α,13- and 11β,13-dihydrosalonitenolide, and the lignans arctigenin, pinoresinol and 7′(S)-hydroxyarctigenin. The latter compound is described for the first time as a natural product. The aerial parts of Centaurea pabotii yielded 11,13-dihydrodeacylcynaropicrin, aguerin A and a new guaianolide related to cynaropicrin.