Late in the 1965–66 NHL season, Smith played two games with the Toronto Maple Leafs, winning one of them and posting a 1.94 goals against average.

From 1967 to 1969 he played 85 games with the Tulsa Oilers, Rochester Americans, and Baltimore Clippers minor league teams before joining the Pittsburgh Penguins, being claimed from the Toronto organization in the NHL Intra-League Draft on June 11, 1969.

Smith was later called up as the backup to Terry Sawchuk for games four and five of 1967 Stanley Cup Finals, due to an injury to Johnny Bower.

Smith also played for the Pittsburgh Penguins, Detroit Red Wings, Buffalo Sabres, Hartford Whalers and Colorado Rockies.

Smith was to replace injured goalie Gerry Desjardins for a game against the Minnesota North Stars, and Buffalo had also called up Don Edwards.

Less than an hour before game time, Buffalo general manager Punch Imlach ordered Sabres coach Floyd Smith to play Edwards instead.

[1] After the national anthem, Smith stepped off the bench, saluted Buffalo owners Seymour and Northrup Knox and headed for the dressing room.

Smith was traded by the Red Wings to Buffalo for future considerations, on March 10, 1975, then signed as a free agent by New England on August 15, 1977.

Subjects would include sports, such as in his 1997 novel The Parade has Passed, featuring a WHA forward who hitchhikes to the funeral of his former coach, who had died in a brawl.

In 1998, Smith used the $34,000 of pension benefits he'd received as part of the NHL's settlement with former players to produce Confessions to Anne Sexton at the Alumnae Theatre on Berkeley Street in downtown Toronto.