Bailey was appointed as Twenty20 captain of the Australian national team in 2012, succeeding Cameron White prior to the two match series against India that ended 1–1.

Bailey was first selected to play for Tasmania in 2005/06, due to injuries to regular players, and he was given an extended stint in the first-class team, scoring 778 Pura Cup runs, including three centuries, and earning a second invitation to the academy.

In February 2011, Bailey led Tasmania to a five wicket Sheffield Shield win over Victoria where he scored an unbeaten 160.

In the 2011/12 Ryobi Cup final in Adelaide, Bailey showed he is made of stern stuff; he scored 101 and was out in the last over.

In 2016, Bailey was signed by the Rising Pune Supergiants, a new Indian Premier League team, as a replacement to Faf du Plessis who was ruled out of due to a finger injury.

[14] In June 2019, he was selected to play for the Montreal Tigers franchise team in the 2019 Global T20 Canada tournament.

[15] In early 2010, Bailey was called up for the ODIs in New Zealand when Michael Clarke returned home for personal reasons – but did not win a cap.

When he did, he did so as captain of the Australian national Twenty20 team, succeeding Cameron White prior to the two match series against India,[18] which ended 1–1.

[19] When he walked out as leader for the T20 at Sydney's Stadium Australia and the match at the MCG, Bailey was in charge of a new-look side.

The fast-bowling allrounder James Faulkner was on his debut, the batsman Travis Birt had earned a recall nearly two years after his last international appearance and Brad Hogg had returned after retiring in 2008.

Bailey's highest score in the shortest format at the time of his appointment had been 60 and he had made only one T20 half-century in the previous three seasons, but he said batting at No.5 opportunities were often limited.

He presided over a 31-run defeat of India in his first match promoting Matthew Wade to the opener's post where he scored 72 .

He still contributed with 32 and his opening replacement Aaron Finch top-scored with 36, but Shaun Marsh at first drop failed to score and the batting was weakened with the allrounders Daniel Christian and James Faulkner left out.

As a result of an injury to Australian captain Michael Clarke, he was included in the first ODI of the series and Bailey top scored with 48 runs in Australia's 204 for 8.

At the start of the Ireland and England tour it was decided that Bailey would not receive a central contract for the 2012/13 season, despite being captain of the national T20I team.

In the fifth ODI Bailey produced some excellent cricket, rounding off his efforts with a 46 from 41 balls to ensuring that Australia posted a troubling total for England.

[24] In November 2013, Bailey became Australia's 436th Test cap in the Ashes and was presented with the baggy green before the start of play by a former captain Mark Taylor.

He was also awarded the Men's ODI Player of the Year at the Allan Border Medal ceremony by the CA in 2014.

[25] On 7 September 2014, George Bailey resigned as the captain of the Australian T20I team to focus solely on the 2015 ODI World Cup.

In August 2017, he was named in a World XI side to play three Twenty20 International matches against Pakistan in the 2017 Independence Cup in Lahore.

[27] During the 2012–13 summer, George Bailey led a one-day Australian team lacking draw-cards David Warner and Shane Watson.