Chaykin died at a Toronto hospital, said his manager, Paul Hemrend. The actor had been battling kidney problems, said Mark McKinney, who produced Chaykin's most recent series, the HBO Canada sitcom "Less Than Kind."
"He was one of our greatest actors," McKinney said. "Maury's an actor of unparalleled gifts. You cannot learn what he had in spades."
In "Dances With Wolves" (1990), Chaykin turned his few minutes of screen time into a breakout role. He portrayed an unhinged cavalry officer who dispatches Kevin Costner's character to a remote fort in Native American country.
Chaykin received considerable attention for starring in the 1994 film "Whale Music" as a faded rock star who finds redemption. He won a Genie Award, the Canadian equivalent of an Oscar, for his portrayal of Desmond Howl, a character based on Beach Boy Brian Wilson.
"A master of the show-stopping cameo," Chaykin created "a dizzying variety of memorable eccentrics," the Canadian weekly Maclean's said in 1994.
His characters included Dustin Hoffman's nosy superintendent in "Hero" (1992) and the slow-witted Southern yokel grilled by Joe Pesci in "My Cousin Vinny" (1992).
A hefty man, Chaykin was often cast in offbeat or gregarious roles. Among his favorite parts were Uncle Arthur in Diane Keaton's "Unstrung Heroes" (1995) and the wealthy entrepreneur in the Canadian film "The Adjuster" (1991).
From 2005 to 2007, Chaykin had a recurring role on the HBO series "Entourage" as Harvey Weingard in a bombastic send-up of the real-life movie executive.
"I have never worked for Harvey Weinstein," Chaykin told the Toronto Star in 2007. "And now I think maybe I never will."
Chaykin was born in 1949 in New York City, the younger of two sons of Irving Chaykin, a City College of New York accounting professor, and his wife, Clarice, a nurse who was a native of Canada.
In the late 1960s, Chaykin studied theater arts at the State University of New York in Buffalo and later trained with Buffalo's American Contemporary Theatre.
Despite appearing in many off-off-Broadway plays, Chaykin struggled to make it as an actor in New York. When offered a role in Toronto's underground theater in 1974, he moved there — and stayed.
Eventually, he found work acting on both sides of the border and appeared in more than 150 film and television projects.
Some of his more recent work included starring in the Canadian TV series "A Nero Wolfe Mystery," which aired from 2001 to 2002, and appearing as a bookie in "Owning Mahowny," a 2003 Canadian-British film.
He is survived by his wife, actress Susannah Hoffman, and daughter, Rose. A first marriage ended in divorce.