The actor died Tuesday evening at New York Presbyterian Hospital. He had been suffering from multiple myeloma and heart disease, said his publicist, Jennifer Plante.
Boyle, whose lovably rude exclamation of "Holy Crap!" was his signature line on the hit sitcom, had a long career in Hollywood.
A member of the Christian Brothers religious order who turned to acting, the tall, prematurely balding Boyle gained notice in the title role of the 1970 sleeper hit "Joe," playing an angry, murderous bigot at odds with the emerging hippie youth culture.
Briefly typecast in tough, irate roles, Boyle began to escape the image as Robert Redford's campaign manager in "The Candidate" and left it behind entirely after "Young Frankenstein," Mel Brooks' 1974 send-up of horror films. The latter movie's defining moment came when Gene Wilder, as scientist Frederick Frankenstein, introduced his creation to an upscale audience. Boyle, decked out in tails, performed a song-and-dance routine to the Irving Berlin classic "Puttin' On the Ritz."
It showed another side of Boyle, one that would be best exploited in the sitcom "Everybody Loves Raymond," in which he played curmudgeonly paterfamilias Frank Barone for 10 years.
"He's just obnoxious in a nice way, just for laughs," Boyle said of the character in a 2001 interview. "It's a very sweet experience having this (success) happen at a time when you basically go back over your life and see every mistake you ever made."
When Boyle tried out for the role opposite series star Ray Romano's Ray Barone, however, he was kept waiting for his audition -- and he was not happy.
"He came in all hot and angry," recalled the show's creator, Phil Rosenthal, "and I hired him because I was afraid of him." But Rosenthal also noted: "I knew right away that he had a comic presence."
Boyle had first come to the public's attention more than a quarter century before, in the critically acclaimed "Joe." He met his wife, Loraine Alterman, on the set of "Young Frankenstein" when she visited as a reporter for Rolling Stone magazine and Boyle, still in monster makeup, asked her for a date.
On television, he starred in "Joe Bash," an acclaimed but short-lived 1986 "dramedy" in which he played a lonely beat cop. He won an Emmy in 1996 for his guest-starring role in an episode of "The X Files," and he was nominated for "Everybody Loves Raymond" and for the 1977 TV film "Tail Gunner Joe," in which he played Sen. Joseph McCarthy.
In the 1976 film "Taxi Driver," he was the cabbie-philosopher Wizard, who counseled Robert DeNiro's violent Travis Bickle.
He did dozens of other films, including "T.R. Baskin," "F.I.S.T.," "Johnny Dangerously," "Conspiracy: Trial of the Chicago 8" (as activist David Dellinger), "The Dream Team," "Monster's Ball," "The Santa Claus," "The Santa Claus 2," "While You Were Sleeping" (in a charming turn as Sandra Bullock's future father-in-law) and "Scooby Doo 2: Monsters Unleashed."
The son of a local TV personality in Philadelphia, Boyle was educated in Roman Catholic schools and spent three years in a monastery before abandoning his religious studies. He later described the experience as similar to "living in the Middle Ages."
He explained his decision to leave in 1991: "I felt the call for awhile; then I felt the normal pull of the world and the flesh."
He traveled to New York to study with Uta Hagen, supporting himself for five years with various jobs, including postal worker, waiter, maitre d' and office temp. Finally, he was cast in a road company version of "The Odd Couple." When the play reached Chicago he quit to study with that city's famed improvisational troupe Second City.
Upon returning to New York, he began to land roles in TV commercials, off-Broadway plays and finally films.
Through his wife, a friend of Yoko Ono, the actor became close friends with John Lennon. "We were both seekers after a truth, looking for a quick way to enlightenment," Boyle once said of Lennon, who was best man at his wedding.
In 1990, Boyle had a stroke and couldn't talk for six months. In 1999, he had a heart attack on the "Raymond" set. He soon regained his health, however, and returned to the series.
Despite his work in "Everybody Loves Raymond" and other Hollywood productions, Boyle made New York City his home. He and his wife had two daughters, Lucy and Amy.
The Associated Press contributed to this report.