FOR THE RECORD: An earlier version of the photo caption with this article misidentified Jim Kiick of the Miami Dolphis as Jim Klick.
A caretaker found Smith at his Baldwin Hills home, police said.
A 6-foot-7, 280-pound defensive end, Smith was the No. 1 NFL draft pick from Michigan State University when he joined the Baltimore Colts in 1967.
He played five seasons for the Colts, which included their upset loss to the New York Jets in Super Bowl III and a victory over the Dallas Cowboys in Super Bowl V. He spent two seasons with the Oakland Raiders and two more with the Houston Oilers before a knee injury ended his career in 1976.
After football, Smith was recruited to the ranks of former professional athletes who appeared as themselves in commercials for Miller Lite beer. He and fellow NFL veteran Dick Butkus were cast as inept golfers and polo players in the TV spots. Smith was also featured solo in one commercial extolling the virtues of the beer, beaming into the camera, "I also love the easy-opening cans," while ripping off the top of the can.
Despite a lucrative contract and widespread popularity, Smith walked away from the job.
"I went back to Michigan State for the homecoming parade last year," Smith told then-Times columnist Scott Ostler in 1986. "I was the grand marshal and I was riding in the back seat of this car. The people were yelling, but they weren't saying, 'Go, State, go!' One side of the street was yelling, 'Tastes great!' and the other side was yelling 'Less filling!'
"Then we go to the stadium. The older folks are yelling 'Kill, Bubba, kill!' But the students are yelling 'Tastes great! Less filling!' Everyone in the stands is drunk. It was like I was contributing to alcohol, and I don't drink. It made me realize I was doing something I didn't want to do."
So he turned to acting in movies and TV, notably playing Moses Hightower in six "Police Academy" movies. He also appeared in a number of TV series, including "Half-Nelson," "Blue Thunder" and "Good Times."
Charles Aaron Smith was born Feb. 28, 1945, in Orange, Texas, and grew up in Beaumont, where his mother was a teacher and his father was his high school football coach.
At Michigan State, Smith became an All-America defensive end for the Spartans, who went 19-1-1 his last two seasons. He also earned a bachelor's degree in sociology.
His brother Tody, a star at USC and in the NFL, later became Bubba's agent. He died at 50 in 1999.
Information on survivors was not immediately available.
Los Angeles Times staff writer Andrew Blankstein contributed to this report.