A 6-foot-7, 250-pound All-American at Michigan State who prompted cries of "Kill, Bubba, Kill!" from Spartans fans, he was the No. 1 pick in the 1967 NFL draft and became a two-time Pro Bowl selection with the Colts before ending his injury-shortened career with the Oakland Raiders and Houston Oilers.
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Smith died Wednesday in Los Angeles at age 66. The cause of death was not immediately announced, but police said they believed he died of natural causes.
"He was a hell of a football player," said Fred Miller, a former Colts defensive tackle and Smith's teammate for five years. "By his second year in the league, once he got his attitude right and worked hard, I don't think there was anyone in the league who could block him.
"We used to prime Bubba all week," Miller continued with a chuckle. "We'd know which offensive lineman he'd be facing in Sunday's game, and we'd say, 'Bubba, he's going to kill you!'
"But it was always the other way around. They hardly touched him."
Recalled Bruce Laird, a former defensive back who played with Smith on the 1972 Colts: "He was basically a freak of nature at 6-foot-7 and 270 pounds. Bubba was the fastest player on the football team for 10 yards."
Ernie Accorsi, who was the Colts public relations director in 1970 and retired three years ago as general manager of the New York Giants, recalled one game in particular when Smith was at his very best as a pass-rusher.
"In the [AFC] championship game in 1970, when we beat the Raiders, 27-17, in Baltimore, he absolutely destroyed the Raiders," Accorsi said. "He knocked [quarterback Daryle] Lamonica out of the game. He was unblockable."
That fierce image helped Smith land in the groundbreaking Miller Lite commercials of the late 1970s that featured an eclectic mix of retired athletes and celebrities arguing about the beer's merits. (Tastes great! Less filling!")
"I had my own way of tackling," he said in the spot. "I used to grab the whole backfield. Then I threw guys out until I found the ball."
At the commercial's end, Smith tore off the top of a beer can while smiling and proclaiming, "I also like the easy-opening cans."
In the "Police Academy" movies of the 1980s, Smith played the role of Moses Hightower, a gentle — if intimidating-looking — giant.
Locally, Smith was also known as a spokesman in commercials for the law firm of Cohen, Snyder, Eisenberg & Katzenberg.
"He was just a good guy," Mike Curtis, a Colts linebacker and four-time Pro Bowl pick, said of Smith. "The movies made him seem like a big galoot. But he wasn't like that at all."
"He was really a gentle, elegant person," Accorsi said. "In the movies, he wasn't acting at all. He was just being Bubba."
Smith was named to the College Football Hall of Fame in 1988. His No. 95 jersey was retired by Michigan State in 2006.