Smith was called up to the Australian Test squad in 2010 to cover for spinner Nathan Hauritz who was in doubt for Boxing Day Test against Pakistan, but Hauritz managed to recover. In the first innings of the last Test of the 2013 Ashes Series at The Oval, Smith scored his maiden hundred, reaching the total in style by hitting a six off the bowling of Jonathan Trott.
By the end of the 2009–2010 domestic season Smith had a first-class batting average of over 50 after just 13 first-class matches. While his first-class bowling average in the high forties was not as impressive, his bowling appeared to be steadily improving following some well-publicised mentoring from Shane Warne. In the final match of the season he took 7 for 64 in the second innings against South Australia.