Smith kicked off his set with 'Nirvana', before surprising fans by welcoming Nile Rodgers on stage for a rendition of 'Together'.
"This is really surreal for me right now to have all these people here," Smith said in response to the size of the crowd, before playing 'Leave Your Lover'.
He then continued with new single 'I'm Not The Only One', 'Restart' and chart-topping hit 'La La La'.
However, it was a performance of 'Lay Me Down', one of Smith's earliest tracks, that received a massive response.
Smith rounded off his set with his number one single 'Money On My Mind' - interpolated with a segment of Cece Peniston's '90s dance anthem 'Finally'- a stripped down rendition of his Disclosure collaboration 'Latch', and his global ballad 'Stay With Me'.
The Killers will headline the Virgin Media stage at V Festival in Chelmsford this evening, while Justin Timberlake will top the bill at Weston Park, Staffordshire.