The 'You Can Call Me Al' hitmaker will headline the Sunday night of the event in Hyde Park, London, on Sunday July 15, performing his classic 'Graceland' album in full.
The performance will come 25 years after the album's original release, and will include Ladysmith Black Mambazo, the South African male choir who appeared on the album. It will be the first time they have performed with Paul in the UK since 1987.
Paul will also be joined on stage by reggae star Jimmy Cliff, performing some of his tracks, including 'The Harder They Come' and 'Too Many Rivers To Cross'.
Hamish Dodds, President and CEO of Hard Rock International said: ''Paul Simon's 'Graceland' is considered to be one of the greatest of albums of all time. We look forward to welcoming Paul Simon to the Hard Rock Calling 2012 stage and celebrating 'Graceland's' 25th Anniversary.''
Also added to the Sunday line up is Alison Krauss & Union Station featuring Jerry Douglas. Lady Antebellum and Creedance Clearwater Revival's John Fogerty have been added to the bill for Saturday (14.07.12), which will be headlined by Bruce Springsteen.
Further announcements, including the Friday night (13.07.12) headline act will follow shortly.
Tickets go on sale on Friday (23.03.12) and are available from www.hardrockcallling.co.uk