Initially he considered following his older brother into the Dominican Order, but he entered the novitiate of the Society of Jesus on April 21, 1681, and was ordained as a priest on October 28, 1695.

Baldinucci himself walked barefoot to each mission assignment,[4] often carried a cross during his preaching, and often wore heavy chains.

His appearances were so popular and well attended that he often found crowds covering the walls of city when he arrived to deliver a mission.

Baldinucci had a particular devotion to the Virgin Mary, and made sure that a copy of miraculous picture of her as the Refuge of Sinners from the Church of the Gesu (Frascati) was carried with him in his travels.

In addition to his preaching, Baldinucci also wrote two courses of sermons for Lent, gathered material for many more, composed a number of discourses, and maintained a long correspondence list.

After suffering from a myocardial infarction in the course of one of his preaching tours, brought on by fatigue, Baldinucci died in the village of Pofi, in the ancient region of Lazio, then part of the Papal States.