Catharanthus roseus (L.) G. Don is one of the most important medicinal plants, mainly due to the presence of anticancer alkaloids. For many years, the phenolic composition of this species remained largely unstudied. Recently, detailed phytochemical studies using the latest analytical techniques have helped understand the complex phenolic profile of this species. Several highly glycosylated flavonoids have been found, mainly quercetin, kaempferol, and isorhamnetin derivatives. Other classes of phenolic compounds, namely benzoic acids and phenylpropanoids have also been described. Additionally, the high content in phenolic compounds turned this plant an interesting source of antioxidants whose activity has already been shown. In this chapter, the tissue-dependant distribution of phenolics, as well as their concentrations and antioxidant activity, will be presented.