The singer was joined on stage by Queen's Brian May for a rousing live rendition of the guitar solo that he recorded with GaGa on the popstar's Born This Way album.
GaGa, dressed in Calderone's white T-shirt and black trousers from the recent 'You and I' video, was accompanied by a group of male backing dancers sporting the same clothing.
The singer delivered the song from behind the piano, stopping at one point to take a swig of beer and eventually climbing on top of the instrument.
Before the performance, GaGa stood alone on the stage to deliver an impassioned monologue as Calderone, smoking and swearing as he critiqued GaGa's persona and criticised the star for leaving him.
"Lady GaGa? She left me. She said it always starts out good and then the guys... get crazy. I did - I got crazy - but she's f**king crazy too," Calderone said.
"She gets out of bed, puts on heels, she comes out of the bathroom dripping wet, she still has the heels on. And what's with the hair? At first it was sexy, but now I'm just confused."
> MTV Video Music Awards 2011: The winners
Watch Lady GaGa as Jo Calderone in the video for 'You and I' below: