Smith's body was found Wednesday at his home in the Baldwin Hills suburb of Los Angeles, said Los Angeles police spokesman Officer Gregory Baek.
He is believed to have died of natural causes, but the coroner's office has not made a final determination, police said.
After a successful NFL career with the Colts, Oilers and Raiders Smith carved out a successful TV career with a series of memorable Miller Lite ads and roles on series like 'Good Times,' 'Blue Thunder' and 'McGyver.'
The 6' 7" Smith played for Michigan State University and entered the National Football League when he was drafted by the Baltimore Colts in 1967.
Aside from winning a Super Bowl with the Colts in 1971, Smith also went on to play with the Oakland Raiders and the Houston Oilers before he retired in 1976, after being twice selected to the Pro Bowl.
He won guest-starring and recurring roles on TV shows spanning three decades, with appearances on series including 'Charlie's Angels,' 'B.J. and the Bear,' 'Taxi,' 'Tales of the Golden Monkey' and 'Married ... With Children.'
Smith also appeared in three episodes of 'Good Times,' playing Marion "Sweet Daddy" Williams' bodyguard, and he landed a starring role in 'Open All Night,' ABC's early '80s sitcom about a dysfunctional family and their convenience store.
The short-lived 1984 series 'Blue Thunder' partnered Smith with Pro Football Hall of Fame defensive star Dick Butkus, with whom he frequently co-starred in a series of hilarious ads for Miller Lite Beer.
But Smith will perhaps be best known for creating the role of Moses Hightower in the 'Police Academy' movie series. He played Cadet (later Sgt.) Hightower, a police recruit who was as soft-spoken as he was physically imposing, in all but one of the movies.
Watch Smith and Butkus in an ad from 1984:
Here's Smith putting his football skills to good use as he goes up against Al Bundy in 'Married ... With Children':