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Nutini's debut album These Streets, produced by Ken Nelson (who has also worked with Coldplay and Gomez), was released on 17 July 2006 and immediately entered the UK album charts at number three.
Many of the songs on the album, including "Last Request" and "Rewind", were inspired by a turbulent relationship with his former girlfriend Teri Brogan, and "Jenny Don't Be Hasty" is a true story about encounters with an older woman.
Nutini became known for singing with his eyes closed during his entire performances.
Throughout 2006, Nutini played a number of sold-out concerts across Britain and performed at a wide variety of venues worldwide, including King Tut's Wah Wah Hut in Glasgow, a TV appearance on Later with Jools Holland, Carnegie Hall in New York, The Montreux Jazz Festival, The Wireless Festival, Oxegen and T in the Park.
He supported the Rolling Stones in Vienna and was invited to appear with them again at the Don Valley Stadium in August 2006 and was also booked to appear at the V Festival and The Austin City Limits Music Festival, Texas, later in 2006, with a European tour in the autumn.
Nutini also performed at the British leg of Live Earth at Wembley Stadium on 7 July 2007, with his set including a cover of "What A Wonderful World", a classic pop tune by Bob Thiele, George David Weiss, and George Douglas.
He performed the following day at T in the Park, in Scotland.