Philothei was born as Revoula Benizelou in Athens on November 21, 1522, to the illustrious and wealthy Benizelos family.

The family wealth gave her the opportunity for charitable work, and while still a young woman she had gained the respect and love of the community.

One of her more controversial activities was to buy the freedom of Greeks taken as slaves by the Ottoman Turks, especially women taken to the harems.

Despite being hunted by the Turks, she helped them escape secretly to Tzia, Andros, Aegina and Salamina, where they were safe.

[2] In a 22 February 1583 letter to the Venetian Gerousia, Philothei asked for monetary support to pay off her debts from ransom money, duties, bribes, and taxes that she owed to the occupying Turks.

Her monasteries were frequently plundered, and the farming and agricultural program, which were a basic source of sustaining her work, devastated.

On 3 October 1588, four Ottoman mercenaries broke into the monastery at Patisia during the evening vigil service and beat her severely.