The rich and diverse flora of Armenia has been used for medicinal purposes for at least 3000 years. The relevant literature in Armenian, English, and Russian revealed a vast array of used medicinal plants, some of them unique to the Caucasus region. The usage of medicinal plants confirms the position of Armenia as a country at the crossroads of Asia and Europe because of its traditional usage of medicinal plants from both continents. Literature data in Armenian, English, and Russian on medicinal plants of Armenia were mainly obtained using various electronic databases. From all available sources, 320 Armenian medicinal plant species were extracted with their botanical and local names and traditional uses. The use of medicinal plants by the Armenian people is systematically compiled, including the used plant organs and preparations and the ailments for which the various taxa are/were used. Medicinal plants of Armenia are represented for both wild and cultivated species. Some of the taxa used are unique to Armenia or the Caucasus region, while many other species are also used in various other countries. Some of the species from traditional Armenian medicine are currently being studied using modern methods.