Smith began his professional career with the Negro league Birmingham Black Barons, where he was selected to play in the East–West All-Star Game in 1958 and 1959.

In 1963, playing for the Triple-A Syracuse Chiefs, he led the International League in winning percentage (.875) with a 14–2 won/loss mark, and posted a 2.11 earned run average.

He had compiled a 1–4 record with an earned run average of 2.84 with the Angels in 31⅔ innings pitched when Halo manager Bill Rigney shifted Smith to the outfield to get his bat in the lineup on a daily basis.

[2] The pinnacle moment of Smith's 245-game stint with the Cubs was his one-out two-run walk-off homer to the right-field bleachers off Barry Lersch in an eleven-inning Opening Day 7–6 win over the Philadelphia Phillies at Wrigley Field on April 8, 1969.

His record as a pitcher was 2–4 with a 3.10 ERA in 29 games; in 61 innings pitched spread over three MLB seasons, he allowed 60 hits and 24 bases on balls, with 39 strikeouts.