Three new phenolic bisbenzylisoquinoline alkaloids, limacine, limacusine, and cuspidaline, were isolated from Limacia cuspidata (Miers) Hook. f. et Thorn. (Menispermaceae) collected in Borneo. Limacine (I) is enantiomeric with fangchinoline, as its NMR and IR spectra are superimposable with those of fangchinoline except for the sign of specific rotation. Limacusine (II) was structurally assigned: methylation with diazomethane afforded O-methyl limacusine identical to N-methyldihydroepistephanine-B antipode; NMR analysis showed no methoxyl signal at 7-position (indicating hydroxyl at 7-position); mass spectrometry provided further evidence. Cuspidaline (IV) was characterized by O-methylation to O,O-dimethylcuspidaline (identical to O-methyldauricine) and cleavage studies yielding two coclaurine-type bases. The biogenetical relationship between these alkaloids is that intramolecular dehydrogenative coupling of cuspidaline (IV) gives rise to both limacine (I) and limacusine (II).