In August 1966, Smith signed for Rangers for a then Scottish record transfer fee of £55,000. He made his debut on 13 August in a Scottish League Cup match versus Hibernian. He would stay at the club until in 1969 and make 68 appearances and score 26 goals, including playing in the 1967 European Cup Winners' Cup Final. Indeed, in that season he was top scorer for the club with 23 goals.