The best actor award was split between Philip Seymour Hoffman and Joaquin Phoenix for The Master.
Inspired by Scientology founder L Ron Hubbard, the film also picked up the Silver Lion prize for best director.
Directed by Paul Thomas Andersen, The Master tells the story of a sect leader who takes a war veteran under his wing.
Hoffman, who also collected Phoenix's award, said: "Joaquin Phoenix is a life force in this film ... and I kind of rode that life force and that was my performance.
"It was really riding his life force because it was something that was untameable and my job was to try to and it was almost impossible, which is kind of the movie."
He also praised Anderson, who was not at the ceremony, calling him: "Friend first, collaborator second. And he happens to be one of the great film-makers."
Philip Seymour Hoffman collected all the awards on behalf of the film
Pieta, directed by Kim Ki-duk, centres on a debt collector who is forced to examine his life when a woman turns up claiming to be his mother.
On accepting his award, Ki-duk sang a song to the audience while thanking the jury.
Speaking after, he said: "This is a song that we Koreans sing when we are sad, when we feel alone, when we feel desperate, but also when we're happy."
The Venice jury, which was headed by US director Michael Mann, picked Hadas Yaron for best actress for Fill the Void, a film delving into the life of an ultra-Orthodox Jewish community.
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