Smith played for Tranmere Rovers since she was a teenager, but after years of fielding several offers from top clubs around the country, she signed on for Leeds United (known as Leeds Carnegie from 2008 until 2010) in the summer of 2002.
Following the failure of Leeds' bid to join the FA WSL, Smith signed for Lincoln Ladies in August 2010. In December 2011 Smith joined Doncaster Rovers Belles, who had tried to sign her on two previous occasions. Belles manager John Buckley described the capture of Smith as "a tremendous coup for the club". Smith scored on her Belles debut in a 2–1 FA Women's Cup win at Barnet, but was later carried off with damaged cruciate and medial ligaments. When she was subsequently ruled out for at least nine months, Buckley rued "a disaster for Sue and a disaster for the club."
Smith made her England debut as a 17–year–old substitute in February 1997, scoring in a 6–4 friendly defeat to Germany at Deepdale in Preston. One of her brightest England moments was scoring a hat-trick of tremendous goals in a home friendly against Spain in March 2001.
She has twice won the Nationwide International Player Of The Year award – in 1999 and 2001. In 1999 she was also voted Players' Player of the Year.
Before winning the 1999 awards, Smith represented her country when she was picked to play in a FIFA XI against the USA in a showpiece match in San Jose.
She made her domestic comeback at the start of the 2002–03 season after suffering a broken leg and torn ligament damage after a training ground accident in February, and after featuring in the series of friendlies in the build-up to Euro 2005, narrowly missed selection in the final 20.
In 2000, Smith and her Tranmere team-mates featured in a television advert for Daz washing powder alongside Julian Clary. Smith was later a regular contributor to the Yorkshire Evening Post's women's football section, and also offered her views and commentary skills for BBC sport, most recently Smith appeared alongside Manchester United'sWayne Rooney in his three-part Sky1 show 'Street Striker'.