In the early 1950s Ortolani was founder and member of a well-known Italian jazz band. He wrote his first score was for Paolo Cavara and Gualtiero Jacopetti's pseudo-documentary Mondo Cane, whose main title-song More earned him a Grammy and was also nominated for an Oscar asBest Song. The success of the soundtrack of Mondo Cane led Ortolani to score films in England and the United States such as The 7th Dawn (1964), The Yellow Rolls-Royce (1964), The Glory Guys (1965) and The Spy with a Cold Nose (1966). Another renowned track was his main-title for the movie O Cangaceiro (1970).
Ortolani scored all or parts of over 200 films, including German westerns like Apache's Last Battle (Old Shatterhand, 1964) and a long series of Italian giallos, spaghetti westerns, Eurospy films, Exploitation films and mondo films. Notable films scored by Ortolani include Il Sorpasso(1962), Io ho paura (1977), Castle of Blood (1964), Anzio (1968), The Bliss of Mrs. Blossom (1968), Sette orchidee macchiate di rosso (1972), Africa Addio (1966), Addio Zio Tom (1971), House on the Edge of the Park (1980), Cannibal Holocaust (1980), and the first series of La Piovra(1984).
More recent scores were featured in Grand Theft Auto: London, 1969 (1999), Kill Bill: Vol. 1 (2003), Kill Bill: Vol. 2 (2004), Drive (2011) and Django Unchained (2012).
Ortolani died on 23 January 2014 in Rome, aged 87.