Natural products remain today an important source of bioactive molecules to be used in human therapeutics. This interest arises mainly from the chemical diversity found in Nature and the ability of several organisms to synthesize a number of molecules whose complexity hinders their total or semi synthesis.

Catharanthus roseus (L.) G. Don (formerly Vinca rosea L.) is one of the most studied medicinal plants due to the accumulation in the leaves of the bisindole monoterpenic alkaloids vinblastine and vincristine, which were the first natural anticancer products to be clinically used. Together with a number of semisynthetic derivatives, these compounds are universally known as the Vinca alkaloids, which are still among the most valuable agents used in the treatment of cancer.

In the past few years, a number of studies focusing other biological properties of this species have emerged. In particular, the antioxidant activity and acetylcholinesterase inhibition of some of its primary and secondary metabolites have showed that, besides anticancer alkaloids, there might be an interest in exploiting this species for other medicinal activities and from a health-promoting point of view.

In this chapter, an update in C. roseus chemistry and bioactivity is presented. New metabolites and new pharmacological properties discovered in the last years using green chemistry approaches are reviewed, and the potential of further exploitation of C. roseus in is discussed.