Rabbi Elio Toaff, who would have turned 100 at the end of April, also helped create a historic moment when he invited then-Pope John Paul II to pray with him in Rome's synagogue in 1986; it was the first visit in modern time by a pontiff to a Jewish temple.
In a letter expressing his condolences, Pope Francis said Rabbi Toaff had won widespread "esteem and appreciation for his moral authority, together with his profound humanity."
"I remember with gratitude his generous commitment and sincere openness to promoting dialogue and close relations between Jews and Catholics, which saw a significant moment in his memorable meeting with St. John Paul II in Rome's synagogue," said the pope's letter, addressed to Rome's Chief Rabbi Riccardo Di Segni.
Born in Livorno, Rabbi Toaff served from 1951 to 2001 as Rome's chief rabbi, heading the Jewish community there soon after Italy's liberation from Nazi occupation and Italian Fascist forces, who deported more than 2,000 Roman Jews.
The Vatican newspaper said he made an "invaluable contribution" to fostering mutual understanding and friendship between Jews and Catholics "in order to overcome a much too long history of rivalry and animosity, conflict and persecution," and he aimed for a common future respectful of differences.
His early home life was an example of religious harmony as his father was friends with a number of Catholic clergy and their housekeeper was Catholic, the newspaper said. The father made sure the housekeeper was free to go to Mass every Sunday and she made sure the children said their evening Jewish prayers when she'd put them to bed, it said.
"Therefore, it was at home, and ever since he was a child, that Toaff lived and learned the spirit of openness that would accompany him his whole life," the newspaper said.
St. John Paul held Rabbi Toaff in such high esteem he mentioned "the rabbi in Rome" in his spiritual testament. After the pope died in 2005, Rabbi Toaff was one of the first to pay his respects.