 On 27 November 1660 he was admitted into the Carmelites at the convent of Cerignano in Fivizzano alongside his brother Tommaso.The two brothers returned home for several months before receiving the habit in Fivizzano, and then deciding to go to Siena to the convent of San Nicola for the novitiate (their father escorted them); Paoli assumed the religious name of "Angelo" in honor of his father.He made his vows on 18 December 1661 and then spent a prolonged period doing his philosophical and theological studies in both Pisa – at the convent of Santa Maria del Carmine – and Florence.