The presence of theobromine (up to 0.14%) and of caffeine (up to 0.76%) has been established for the first time in beans from two populations of Coffea lancijdia (A320 and A405) and in one population of C. kianjavatensis (A213). This indicates that the Mascarocoffea, once thought to be purine-free, includes some members storing methyl xanthines in seeds, but the virtual absence of caffeine from another C. kianjavatensis (A602), and of both caffeine and theobromine from three populations of C. homollei (A574, A743 and SZlOS) indicates the biochemical diversity of these taxa.