The Tennessee band will bring their Come Around Sundown LP to the event on Friday, June 10, in the middle of their own tour of outdoor venues.
Festival promoter John Giddings said: "We are proud to bring one of the world's biggest rock bands to the island on our tenth anniversary. It is an incredible way to start the weekend, I can't wait!"
Isle of Wight Festival takes place from Friday June 10 to Sunday June 12, 2011. Tickets go on sale this Friday, November 19.
Last year's event was headlined by Jay-Z, The Strokes and Paul McCartney.