In 2010, Larkham returned to the Brumbies ahead of the 2011 Super Rugby season to take up the role of attack coach. He worked under the head coach of Tony Rea who left the franchise at the end of that season. Larkham and newly appointed head coach Jake White made a formidable duo, as during the 2012 Super Rugby season, the Brumbies went from being the fourth best Australian franchise to the second best behind the Queensland Reds. Larkham's attacking influence saw the Brumbies pick up 5 bonus points wins, and an overall better point difference in favor of for. He guided Matt Toomua and Christian Lealiifano to world class fly-half options, which helped the Brumbies secure the top Australian conference position during the 2013 Super Rugby season, finishing second overall losing in the final to the Chiefs 27–22. In 2014, Jake White dramatically resigned as head coach, with Larkham and Laurie Fisher being appointed joint coaches for that season. They finished second in the Australian conference and fourth in the standings after the regular season. They faced the Waratahs in the Semi-final, losing 26–8 in Sydney.