Behind the church, which dates from the 13th Century, are found the administrative offices of the Holy Synod of the Church of Greece. In front of the Catholicon (the main church), lies the tomb of the Teacher of the Hellenic Nation, Constantinos Oikonomou.

In the beginning, the Byzantine-era monastery was called "Coucopouli" in honor of its founder, which was a dependency of the monastery of St. John the Forerunner in Kareas, Ymmitos, but later the monks moved in for safety reasons. In 1673, the monk, doctor, and philosopher Parthenios Petrakis from Demetsana, Peloponnese, came to the monastery and radically rebuilt it. Since then, the premises bears his name. During the Hellenic War of Independence (1821-1829), the Turks plundered the monastery. Following the establishment of the Greek State, Petraki was utilized as an armory as well as a military hospital. After 1922, it housed refugees from Turkey and, during the Axis Occupation of Greece, it provided food to children in need.

The entire property was gradually became entrusted to believers, thus making the monastery one of the greatest benefactors of Athens. With donations from its former guardians, the hospitals of Evangelismos, Sotiria, and Syngrou were erected. Moreover, the Rizarios Ecclesiastical School, the Academy of Athens, the Polytechnical University, the Gennadios Library, and more were established. In its official capacity, the Catholicon of the Monastery was proclaimed the Synodal Chapel by the decision of the Standing Holy Synod of the Church of Greece. Petraki Monastery consists of a total of 20 ecclesiastical dependencies, as well as historical and religious monument located in the Attica region.

Today there are nearly 20 monks living on the premises. It celebrates on November 8th the Feast of the Bodiless Powers, and on February 7th, memorial services are held for the soul of the founder First Abbot Parthenios Petrakis.

The holy services of the Petraki Monastery are broadcast live daily from the radio station of the Church of Greece, and the Divine Liturgy is performed daily for believers from 06:00 to 08:15.