The singer will perform his debut single 'Is This Love' and new tracks from his first album Misty Eye at the music festival, which takes place at various venues across Brighton between May 10 and 12.
Alabama Shakes, Grimes, Madeon, Maximo Park, Niki & The Dove, Ren Harvieu and Spector are among the acts previously confirmed to play this year's event.
Tickets for Great Escape 2012 are on sale now and can be purchased through the festival's official homepage.
Meanwhile, Grimshaw's debut single 'Is This Love' will be released through RCA on June 3. His first studio album Misty Eye will follow on August 13.
Watch the music video for Aiden Grimshaw's 'Is This Love' below: