It was founded in the 11th century, at the time of emperor Andronikos II Palaiologos. In the 13th century, as a result of the activity of pirates and Latins, Karakallou was totally deserted. It was rebuit in the 16th century.
The monastery ranks eleventh in the hierarchy of the Athonite monasteries.
The library holds 279 manuscripts, and about 2,500 printed books.
The monastery has 30 working monks.