Smith was one of the founder members of the Queen's Park club, based in Glasgow. At the inaugural meeting of the club, held on 9 July 1867, he was listed as the club's first captain and treasurer.
In his "Scottish Football Reminiscences and Sketches" written in 1890, David Bone describes Smith thus:
not by any means an impulsive player, but took in the situation quietly; and while no man ever worked harder in the field, or did more for a club, he was not what could be called a brilliant forward. (He) did well in the (1872) international, and considerably helped the eleven to make a drawn battle of it.
By November 1870, Smith had moved to London and, although he retained his membership of Queen's Park, was also a member of South Norwood, for whom he played in the FA Cup. A Scottish XI had played an English XI in the first (unofficial) international match in March, which ended in a 1–1 draw. After criticism that the first match featured only London-based Scotsmen, the organiser, C. W. Alcock, had written to Scottish newspapers in an effort to attract players from north of the border. As one of the few active football clubs in Scotland at this time, Queen's Park decided to send a representative but were put off by the cost of sending a player to London; as a result, Smith was nominated to represent the club.
The match ended in a 1–0 victory for the English, with the only goal coming from R. S. F. Walker. Despite further criticism in Scotland of the lack of players from outside London, further matches were arranged twice a season; Smith retained his place for the matches played on 25 February 1871 and 18 November 1871, being listed as captain in the November 1871 match. Smith, along with his younger brother James, was named amongst 16 selected players in the publicity for the match played on 24 February 1872, but neither actually played.