This chapter discusses isolation of new monomeric Aspidosperma alkaloids and those of Melodinus, Tabernaemontana, and Ochrosia. This is followed by successive discussions of the chemical and extensive synthetic reactions carried out on these alkaloids. Finally, the recent use of X-ray crystallography and 13C NMR techniques in the structure elucidation of these alkaloids is summarized. Several reviews are pertinent to the discussion. The Swiss group has discussed a different approach to the classification of indole alkaloids along biogenetic grounds and has described the biogenetic routes in fascinating detail. In a complementary review, this author has discussed comprehensively the biosynthetic experimentation on monoterpenoid indole alkaloids. In addition, Kapil and Brown have reviewed the closely related area of nitrogenous glycosides in this volume. Gabetta has summarized the indole alkaloids isolated between 1968 and mid-1972, and Aliev and Babaev have discussed the physical properties of the many Aspidosperma-type alkaloids isolated from Vinca species. © 1979, Academic Press, Inc.