The Kill Bill star will preside over the panel of acclaimed filmmakers, critics and actors for the film festival’s second most prestigious award.
Thurman and the panel will have to pick a winner from a programme of titles including Michel Franco’s April’s Daughter, Kiyoshi Kurosawa’s Before We Vanish and Mathieu Amalric’s Barbara.
The US actress, 46, was a member of the main competition jury when it was headed up by Robert De Niro back in 2011.
Directors competing for the Palme D’Or this year include Todd Haynes, Yorgos Lanthimos, Lynne Ramsay, Sofia Coppola and Michael Haneke.
Stars including Nicole Kidman, Colin Farrell, Joaquin Phoenix and Adam Sandler are set to walk the red carpet on the Croisette.
A total of 18 new films will screen in competition, including Lanthimos’ eagerly-awaited The Killing of a Sacred Deer and Haynes's Wonderstruck.
This year’s festival will be opened by Arnaud Desplechin's Ismael's Ghosts, starring Marion Cotillard.
Netflix will makes its festival debut, with two of its original films being shown this year.
Bong Joon Ho’s monster movie Okja and Baumbach's The Meyerowitz Stories will both screen in the official competition.
The 70th Cannes Film Festival kicks off on May 17.