The opening bands were Deerhoof and then Fallou Dieng. Deerhoof can best be described as a four-piece super-electic San Franciso band experimenting in wildly varying rock timelines and beats with high-pitched vocals from their asian female vocalist. I don't think the crowd liked them much but I kind of liked a couple songs because they reminded me of The Flaming Lips in their earlier, more raw formative years.
Fallou Dieng is a great Senegalese nine-piece band with a great rhythmic African sound. They were tapped at the last minute to replace Youssou N'Dour who could not make the gig for some reason.
Gnarls Barkley was awesome as expected and really rocked the bowl. They played alot of their best songs as well as a cover of "Reckoner" by Radiohead for their encore. Alot of people don't know Gnarls Barkley isn't some actual person, but it's just a name. The lead talent is Danger Mouse who played piano and Cee-lo Green who is the vocalist. Of course they "had" to play "Crazy" as they were "contractually obligated" as they put it.
Here's a great article that goes into more depth about the concert.