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From 1996 to 1999, Simon was a guitarist and keyboardist for The Verve. He was brought in to replace lead guitarist Nick McCabe after the band's first short-lived split, but remained with them when McCabe returned. Their third album was 1997's highly acclaimed Urban Hymns. He played on many of their hits from that time such as The Drugs Don't Work, Bittersweet Symphony and Sonnet. The Verve disbanded in 1999 and later reformed in 2007, this time without Simon. By 2009 they had disbanded again.
Following Graham Coxon's departure from Blur in 2002, he was recruited as guitarist for some of the band's live performances. He continued the relationship formed with frontman Damon Albarn by contributing guitar to Gorillaz' 2005 album Demon Days. Tong also contributed Guitar to Gorillaz' 2010 album Plastic Beach.
Erland and the Carnival/The Good, the Bad & the Queen; 2006–present
In July 2006, it was reported that Tong would again be working with Damon Albarn. NME reported that Albarn had foregone plans to record a solo album and instead formed a new unnamed group which featured Tong with Albarn, former Clash bassist Paul Simonon and drummer Tony Allen. The band released their first album The Good, the Bad & the Queen on 23 January 2007, with the single "Herculean" in October 2006. The album has enjoyed very good reviews and a second single, "Kingdom of Doom", was also released in January 2007 as part of their pan European tour.
Tong also set up a record label with Youth (of Killing Joke) called Butterfly Recordings. The first acts to be released are Indigo Moss and Duke Garwood along with a compilation entitled "What the Folk".
In 2012 Simon contributed to the recording of the Dr Dee soundtrack, written by Damon Albarn, which was released on 7 May 2012.