His greatest success as a track cyclist came in the 2004 Summer Olympics in Athens, where he won gold medals in the sprint and Keirin events.

Following Bayley's failiure to win a medal at the World Cup round in Sydney in December 2007, he was criticized by Martin Barras, the national coach, for not developing his tactics. He was still employing the same final kick which achieved success in Athens, the opposition had learnt to attack early to counter this.