Smith's body was found just before 1 p.m. on Wednesday at his home in Baldwin Hills.
The top overall pick in the 1967 draft after a sensational career at Michigan State, the 6-foot-7 Smith spent five seasons with the Baltimore Colts and two seasons each with Oakland and Houston. He won the 1971 Super Bowl with the Colts.
"I'm saddened by it," Colts owner Jim Irsay said. "I remember my first training camp in 1972 in Golden, Colo. I spent a lot of time with him there. He was a great guy. He was a giant, the biggest player on the field."
But comedy fans may best remember him for his role as police recruit Moses Hightower in the "Police Academy" movies. He also appeared in such television series as "Good Times" and "Charlie's Angels," and was a regular in the ground-breaking Miller Lite commercials featuring retired players.
Police say it appears Smith died of natural causes, but an autopsy is still pending.
The Associated Press contributed to this story.