The musicians will work alongside Oscar-winning British filmmaker and producer Danny Boyle, who is serving as the July 27 event's artistic director.
Underworld and Boyle previously collaborated together on Boyle's films "Trainspotting," "A Life Less Ordinary," "The Beach" and "Sunshine." In 2010, they got together again to work on the National Theatre production of "Frankenstein."
"Appointing Underworld to direct the music in the Olympic Opening Ceremony is the final piece of the jigsaw for the team of leading British creatives who will deliver the ceremonies," Boyle said in a statement Wednesday. "What's interesting about working with them is how much broader their taste is than you might imagine. With 'Frankenstein' we really saw how far we could take a broader approach than we'd used together on the films."
"The 'Frankenstein' project at the National Theatre was our opportunity to test ourselves as writers and music directors in a completely new environment -- Danny asked us to take responsibility for every aspect of the sound and music and encouraged us to draw on a wide musical palette. It was a challenging piece of work with its roots in classic literature, that turned out to be the most fun I've ever had," Smith added.
"We want to leave people with a musical memory of the show rather than a purely visual one. It's a great honor to be asked to do this and one we're taking very seriously -- it's certainly not something we'll get the chance to do again," Hyde said.
2014: The Year in Fashion [PHOTOS]
Alanis Morisette debuts new blonde hair