Two Rubiaceae-type cyclopeptides, 6-O-methylbouvardin (1) and the new cyclopeptide 5β-hydroxy-RA-III (2), were isolated from the roots of Galianthe thalictroides. Employing the sulforhodamine B assay, compounds 1and 2were tested in vitro against three cancer cell lines786-0 (kidney carcinoma), PC-3 (prostate carcinoma), and HT-29 (colon carcinoma)and showed GI50values ranging from 0.06 to 1.80 μg mL–1. This is the first report on the isolation of Rubiaceae-type cyclopeptides from a genus other than Rubiaor Bouvardia.