The lands of the Armenians were for millennia located in Eastern Anatolia, on the Armenian Highlands, and into the Caucasus Mountain range. First mentioned almost contemporaneously by a Greek and Persian source in the 6th century BC, modern DNA studies have shown that the people themselves had already been in place for many millennia. Those people the world know as Armenians call themselves Hay and their country Hayots' ashkharh –the land of the Armenians, today known as Hayastan. Their language, Hayeren [Armenian] constitutes a separate and unique branch of the Indo-European linguistic family tree. A spoken language until Christianity became the state religion in 314 AD, a unique alphabet was created for it in 407, both for the propagation of the new faith and to avoid assimilation into the Persian literary world.

Soon after the alphabet's creation, translations of the bible, religious works, and histories written in Greek and Syriac appeared. In many cases, the originals have been lost to the world leaving these important translations for the future. Alongside these, the Armenians began to write their own unique histories which have become vital documents for the study of the neighboring peoples, cultures, and countries.

The Armenian collections of the Library of Congress include a significant number of these works, many of them often deemed rare. The earliest of the Armenian manuscripts in the collections of the Near East Section of the African and Middle Eastern Division is a 1321 Gospel Book [Awetaran] copied in Jerusalem by the Abbot Nersēs. There are also several manuscripts dating from the early to mid-20th century which have not been digitized due to their copyright status but which can be requested in the African and Middle Eastern Reading Room. The Armenian manuscript collection includes religious treatises, bibles, liturgies, palmistry, cookbooks, and calligraphy sheets taken from a 17th century manuscripts.

The first printed book in Armenian was published in Rome in 1512. The Library does not own a copy of it but its collection of Armenian incunabula does own the first complete publication of the bible in Classical Armenian, known as the Oskan bible for its editor, and published in Amsterdam in 1666. The Library's collection of early printed materials includes those published in the major areas of the centuries-old Armenian Diaspora and include religious, historical, and sociological publications.               

While the major portion Armenian rarities are in the Near East Section of the African and Middle Eastern Division, several other divisions include equally rare and vital documents. The Geography and Map Division possesses, for instance, several rare Armenian maps and atlases, while the Prints and Photographs Division is a treasure trove of rare photographs from the late 19th and early 20th centuries. Taken together, these various collections for a major research center for the world of scholars studying this ancient people and language.