The groundbreaking Glasgow group will be unveiling a specially-commissioned-collaboration with Turner Prize nominee Jim Lambie at the "3D Festival" event on 14 and 15 September.
Rising stars Lewis Capaldi and Be Charlotte will also be performing at the event, which is expected to attract up to 20,000 people to the city's new waterfront arena on the museum's opening weekend.
The 3D Festival has been planned by T in the Park and TRNSMT organisers DF Concerts and a special Young People's Collective set up by the team behind Scotland's first design museum.
The Friday night concert will also feature a specially-commissioned dance performance by Dundee-based outfit Shaper/Caper, while special sound and light installations will transform the city's new Slessor Gardens park and Japanese architect Kengo Kuma's building.
Sistema Scotland, the charity which has set up Big Noise youth orchestras across Scotland, including Dundee, will be involved in the second day of the festival, along with the city's celebrated singer-songwriter Gary Clark.
A special limited edition of The Beano comic will be created for the 3D Festival and will only be available at the event.
A two-week ballot will be held for tickets to the Friday night concert, while the Saturday event will be unticketed.
Free entry to the museum, which officially opens on the Saturday morning, will be ticketed on the opening weekend.
V&A Dundee director Philip Long said: "The journey to create V&A Dundee has already captured the imagination of audiences in the city and far beyond, and anticipation is growing towards its opening.
“The 3D Festival provides a unique moment in time to celebrate the new museum, the city and its transformational journey and we’re delighted to have young people at the heart of this special celebration.
“The programme for the festival brings fantastic creative talent together from across Scotland, both established and new, promising an opening event for V&A Dundee that will be unforgettable."
Primal Scream frontman Bobby Gillespie said: "We’re looking forward to performing at the V&A Dundee opening and collaborating with our dear friend Jim Lambie again."
DF Concerts chief executive Geoff Ellis said: "We will see a lot of collaborations over the weekend of 3D Festival – from headliners Primal Scream with visual artist Jim Lambie, to Sistema Scotland with Dundee legend Gary Clark for a unique performance.
“It is indeed an honour to be working in partnership with V&A Dundee to bring this globally significant event from conception through to fruition, highlighting Dundee as a leading city of design."