His movie career started in 1962 with the soundtrack for the Mondo Cane documentary. The main song in the movie, More, sung by Katyna Ranieri (his wife), resulted in an Oscar Nomination in 1964 as “Best Theme Song” and won the Grammy Award as “Best Instrumental Theme”. More went on to be recorded by over a thousand different artists and is one of the most covered songs in music history. Ortolani went on to score many movies for the Hollywood movie studios working, with directors like Vittorio De Sica, Dino Risi, Franco Zeffirelli, Terence Young, and Edward Dmytryk, as well as having long and fruitful artistic associations in Italy with Damiano Damiani and Pupi Avati. His scores include from Mondo Cane, The Easy Life, Anzio, Farewell Africa, The Yellow Rolls Royce, Women of the World, Valachi Papers, Brother Sun, Sister Moon, Ma Quando Arrivano Le Ragazze, La Rivincita di Natale, Il Papà di Giovanna and Una Sconfinata Giovinezza.
In recent years the ever innovative composer wrote a symphony (2001's Sinfonia della Memoria - Symphony of Memory), a ballet (In Una Parte di Cielo) based on the life of Michelangelo, and in 2007 the Musical Il Principe della Gioventù/La Conguira, inspired by the Pazzi conspiracy, the plot by the Pazzi family to overthrow the Medici family as rulers of Renaissance Florence. Having conducted many famous symphony orchestras, he also had a successful tour of Japan with the Vienna Symphony. Ortolani received numerous awards and citations during his life and in 1995 was made a Commendatore of the Italian Republic by President Scalfaro, one of the highest honours that country bestows. In 2006 He received a BMI USA Special Citation of achievement over seven million broadcast performances of “More” and over fifteen hundred different versions recorded by major artists and orchestras, with over 70 million copies sold, and in 2013 was awarded the Lifetime Achievement Award from the World Soundtrack Academy.