<jats:title>Abstract</jats:title><jats:p>A new secondary metabolite, pterocephaline, along with the known cantleyoside, 7α‐morroniside, 3β,5α‐tetrahydrodesoxycordifoline lactam, 5<jats:italic>S</jats:italic>‐5‐carboxyvincoside, sweroside, and loganin have been isolated from the aerial parts of <jats:italic>P. pinardii</jats:italic> (Dipsacaceae). Moreover, cantleyoside‐methyl‐hemiacetal and cantleyoside‐dimethyl‐acetal were obtained as seco‐iridoid artifacts. The structures were elucidated by extensive spectroscopic methods including 1D‐(<jats:sup>1</jats:sup>H, <jats:sup>13</jats:sup>C and TOCSY) and 2D‐NMR (DQF‐COSY, HSQC and HMBC). Monoterpenoid glucoindole alkaloids were encountered for the first time in Dipsacaceae family. Copyright © 2010 John Wiley & Sons, Ltd.