His 2001 single "Let's Roll" was a tribute to the victims of the September 11 attacks, and the effective action taken by the passengers and crew on Flight 93 in particular.
In 2003, Young released Greendale, a concept album recorded with Crazy Horse members Billy Talbot and Ralph Molina. The songs loosely revolved around the murder of a police officer in a small town in California and its effects on the town's inhabitants. Under the pseudonym "Bernard Shakey", Young directed an accompanying film of the same name, featuring actors lip-synching to the music from the album. He toured extensively with the Greendale material throughout 2003 and 2004, first with a solo, acoustic version in Europe, then with a full-cast stage show in North America, Japan, and Australia. Young began using biodiesel on the 2004 Greendale tour, powering his trucks and tour buses with the fuel. "Our Greendale tour is now ozone friendly", he said. "I plan to continue to use this government approved and regulated fuel exclusively from now on to prove that it is possible to deliver the goods anywhere in North America without using foreign oil, while being environmentally responsible.
In March 2005, while working on the Prairie Wind album in Nashville, Young was diagnosed with a brain aneurysm.
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