Having won her first senior national cap in 2005, Sophie Smith played her first major FINA tournament at the 2009 World Championships. She went on to win medals at the 2010 World Cup and World League Finals before being a part of Australia's 2011 World Championship team which finished fifth. Smith played her 150th match for the senior team at the London Olympic Test Event which Australia went on to win.
Having been one of the last players to miss the Beijing 2008 Games squad, Smith made her Olympic debut in London. The Australians opened their campaign with three victories to top their group in the preliminary rounds before beating the Chinese in a penalty shoot-out in the quarter-final. The Aussies were involved in another extra-time thriller in the semi-final, but their long-time American rivals came out on top 11-9. Australia went on to beat Hungary 13-11 to take home the bronze medal.