Knowledge about folk medicines is limited to elder community members of remote communities, like Sete Cidades in the Azores. The Azores, 1300 km west of Portugal, are nine volcanic islands, totalling 2330 km2 of land dispersed by 173,200 km2 in the North Atlantic Ocean. The present study aims to scientifically document the uses of plant species for medicinal purposes, in the Sete Cidades. Twenty-eight community members from 40 to 84 years of age, of whom half were 55 to 64 years old, were interviewed. Twenty-nine taxa were reported as being used for medicinal purposes, ten of which have not been previously reported for ethnomedicinal use in Portugal, with a first record of the use of Morella faya. Leaves were the most used plant part (55%), and decoction the most common preparation mode. The five reported taxa with both the highest use value (0.71–0.25) and relative frequency of citation (0.14–0.11) were Clinopodium menthifolium subsp. ascendens, Aloysia citriodora, Mentha x piperita, Citrus limon and Rosmarinus officinalis. The traditional uses of some of the reported plants are supported by scientific studies, confirming their ethnomedicinal value and the need to preserve local knowledge of folk medicine practices.