This chapter provides an overview of Aristotelia alkaloids including characterization and structural determination, synthesis, biogenesis, pharmacology and applications in folk medicine. The alkaloids isolated from Aristotelia are all indolic, but otherwise have no structural relationship with the only indole alkaloid from Elaeocarpus spp. Like the great majority of known indole alkaloids, they appear to be constructed from tryptamine and a terpenoid unit, but they differ in as much as the latter has not undergone a preliminary rearrangement to an iridoid before incorporation into the alkaloid structure. Peduncularine is the first alkaloid to be isolated from Aristotelia spp., and it differs from others reported subsequently in being very sparingly soluble in cold chloroform. The Aristotelia alkaloids appear to constitute a unique series of indole bases, in which an unchanged terpenoid unit is incorporated into the molecule without preliminary conversion to an iridoid, although, various rearrangements may take place subsequently. © 1985, Elsevier Science & Technology. All rights reserved.