Jones released a single on 19 March 2012, produced by former White Stripes frontman Jack White, called Evil. The single was first made available through independent record shops in 7" vinyl format on 5 March. An exclusive three-coloured vinyl was also sold at only one shop – Spillers Records in Cardiff. The shop, from which Jones bought records as a schoolboy in the 1950s and early 1960s, was founded in 1894 and is listed in Guinness World Records as the oldest record shop in the world.
In March 2012, Jones became a coach on the BBC talent show The Voice UK. Jones was joined by will.i.am, Jessie J and Danny O'Donoghue. He mentored Leanne Mitchell to win the first series. Jones returned to coach in 2013, 2014 and 2015. In August 2015, it was announced that Jones's contract with the show would not be renewed and that he would be replaced by Boy George. Jones criticised BBC executives for "sub-standard behaviour", having not consulted with him and informing him only 24 hours before the official announcement.
In May 2012, Jones released the album Spirit in the Room on Island Records/Universal Music. The track listing included covers of songs by Paul McCartney, Paul Simon, Leonard Cohen and Richard and Linda Thompson, Blind Willie Johnson, Tom Waits and the Low Anthem.
In May 2012, he starred in a one-off television drama titled "King of the Teds" which aired on Sky Arts as part of a series of standalone teleplays for Playhouse Presents.
On 4 June 2012, Jones performed at the Queen's Diamond Jubilee Concert in front of Buckingham Palace, singing "Delilah" and "Mama Told Me Not to Come".
On 18 August 2012, Jones performed a fifty-minute set at the V Festival’s Weston Park site in Staffordshire. On 9 September 2012, Jones headlined at BBC Radio 2's Live in Hyde Park festival.