On 5 March 2009 it was announced that Jones would captain the Welsh international squad against Italy in the Six Nations Championship.
On 21 April 2009 it was revealed that Jones was one of 13 Welsh Internationals in the squad for the 2009 British and Irish Lions tour to South Africa. He scored a try in his debut for the Lions against the Royal XV. He started the First Test and came on as a replacement in the Second and Third Tests.
On 18 January 2010 he was named in the 35 man Wales national Squad for the 2010 Six Nations tournament. During the first 2010 Six Nations game against England, Jones intentionally tripped English player Dylan Hartley, for which he was sent to the sin-bin. During his 10 minutes there, England scored 17 points, and went on to victory. Warren Gatland, Welsh coach was quoted to say "It was absolutely stupid what he has done and to be honest he has probably cost Wales the game today" live on the BBC after the game.
On 23 August 2010, the Ospreys announced that Jones would succeed Welsh team-mate Ryan Jones as club captain for the 2010/11 season. The decision was made, in part, so Ryan Jones could concentrate on the national captaincy during a busy World Cup year.
On 30 April 2013, Jones was selected for the 2013 British and Irish Lions tour to Australia and was in contention for the captaincy which went to fellow Welsh player Sam Warburton. However, due to Warburton's tour-ending injury in the second test, Jones was selected as captain for the deciding third test in Sydney, which the Lions won 41-16. This made him the first substitute captain to lead the Lions to victory in the final test of a series since 1904.