The subfamily Barnadesioideae (Asteraceae) constitutes a group of spiny plants that are entirely restricted to South America and currently encompasses 92 species distributed in nine genera. Barnadesioideae is particularly interesting because this subfamily constitutes the sister group of all other Asteraceae, and provides insights into the early evolution of Asteraceae. The present work summarizes the current knowledge of the chemistry and medicinal uses of Barnadesioideae. The up-to-date phytochemical profile of Barnadesioideae is composed of phenolic compounds, flavonoids, and triterpenoids, representing 39 different compounds described in 45 species of the subfamily. The presumable absence of sesquiterpene lactones—the typical Asteraceae taxonomical markers—in members of Barnadesioideae is also discussed. A few members of the genera Barnadesia, Dasyphyllum, and more frequently, Chuquiraga, are reported in the traditional medicine of Argentina, Brazil, Bolivia, Chile, Colombia, Ecuador, and Peru, where they are known for their antitussive, expectorant, anti-inflammatory, and many other properties. Chuquiraga jussieui, Chuquiraga spinosa, and Chuquiraga weberbaueri are species frequently sold in medicinal plant markets of Ecuador and Peru, where they are commonly recommended for the relief of genitourinary and reproductive disorders in women and men. Some phytopharmaceuticals containing C. spinosa are also marketed in Europe and North America. Further phytochemical studies on the members of Barnadesioideae would be of great interest for the chemotaxonomy of the family Asteraceae. Moreover, profiling the phytochemical composition of those medically important Barnadesioideae would support their uses in traditional medicine.

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