In 1947 Toaff served as a rabbi in Venice and in 1951 he became the Chief Rabbi of Rome.
One of his children is Israeli-Italian professor Ariel Toaff.
On May 17th 2012 he has been awarded the Prize Culturae within the Italian National Festival of Cultures in Pisa
Upon the 1958 death of the war time Pope Pius XII, Toaff, as Chief Rabbi of Rome, paid tribute to the late Pontiff, saying: "Jews will always remember what the Catholic Church did for them by order of the Pope during the Second World War. When the war was raging, Pius spoke out very often to condemn the false race theory."
On 13 April 1986, Toaff was greeted by, and prayed with, Pope John Paul II during an unannounced visit to the Synagogue of Rome. On April 7, 1994, Toaff co-officiated at the Papal Concert to Commemorate the Shoah at the Sala Nervi in Vatican City, along with Pope John Paul II, and the President of Italy Oscar Luigi Scalfaro.
- Perfidi giudei, fratelli maggiori, 1987
- Essere ebreo with Alain Elkann, 1994
- Paul O'Shea; A Cross Too Heavy; Rosenberg Publishing; 2008; p. 36
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