Irene Papas was born as Irini Lelekou (Ειρήνη Λελέκου) in Chiliomodi outside Corinth, Greece. She sits on the board of directors of the Anna-Marie Foundation along with members of Greece's deposed royal family.

Papas began her early career in Greece (she was discovered by Elia Kazan), achieving widespread fame there, before starring in internationally renowned films such as The Guns of Navarone and Zorba the Greek, and critically acclaimed films such as Z and Electra. She is a leading figure in cinematic transcriptions of ancient tragedy since she has portrayed Helen in The Trojan Women, Clytemnestra in Iphigenia, and the eponymous parts in Electra and Antigone. She appeared as Catherine of Aragon in the film Anne of the Thousand Days, opposite Richard Burton and Geneviève Bujold in 1969. She co-starred in The Trojan Women with Katharine Hepburn, who once said that Papas was "one of the best actresses in the history of cinema".[citation needed]

In 1977, she starred in the film Mohammad, Messenger of God (also known as The Message) about the origin of Islam, and the message of prophet Mohammad. Her last film appearance was in Captain Corelli's Mandolin. She is currently working in theatre in Portugal.

In 1979, Papas collaborated with composer Vangelis in an electronic rendition of eight Greek folk songs, issued as a record called "Odes". They collaborated again in 1983 for "Rhapsodies", an electronic rendition of seven Byzantine liturgical hymns.[citation needed]

In 1982, she appeared in the film Lion of the Desert, together with Anthony Quinn, Oliver Reed, Rod Steiger, and Sir John Gielgud.

One of the more unusual moments in Papas' career came in 1970, when she guested on the album 666 by Greek rock group Aphrodite's Child on the track "∞" (infinity). She chants "I was, I am, I am to come" repeatedly and wildly over a percussive backing. The track was considered lewd by record company executives, and resulted in the album being withheld from release for two years by Polydor Records. Upon its release in 1972, the song caused some furor in Greece and was again accused of lewdness and indecency by Greek religious figures and government authorities.

In 1979, Polydor released her solo album entitled Odes, with music performed (and partly composed) by Vangelis Papathanassiou (also previously a member of Aphrodite's Child). The words for the album were co-written by Arianna Stassinopoulos (Arianna Huffington).

In 1986 Papas released a further album in collaboration with Vangelis, entitled Rhapsodies (Polydor CD 829 413-2).