The hip-hop duo - who reunited at the Coachella Festival in April - marked their first performance in the UK in several years with a slew of old favourites including 'Ms. Jackson' and 'Roses', which had the crowd singing along.
Sunday headliner Bruno Mars, meanwhile, put on an electric show that earned high praise from fans in attendance - including A-list actor Hugh Jackman - and his incredible stage show, complete with fireworks, marked a stark contrast to the controversial performances by Kanye West on the previous two nights.
The 36-year-old rapper was booed for deviating from his music into long rants on both Friday (04.07.14) and Saturday night (05.07.14), but Bruno, 28, kept the 100,000-plus crowd on side by not only performing his own hits, but interspersing his set with classics such as Led Zeppelin's 'Whole Lotta Love', Michael Jackson's 'Rock With You' and Ginuwine's 'Pony'.
Bruno, who alluded to his humble beginnings performing in London clubs, regaled the crowd with hits including 'Just the Way You Are', 'Treasure' and 'Grenade' before closing the show with 'Locked Out of Heaven' and 'Gorilla'.
British pop star Ellie Goulding also took to the main stage at Finsbury Park, London, performing 'Burn' and 'Goodness Gracious' for a crowd that included her pal Cara Delevingne and The Saturdays members Frankie Sandford and Vanessa White. Following her early evening set, Ellie and supermodel Cara jetted across town to Hyde Park to watch her boyfriend Dougie Poynter perform with McBusted a the Barclaycard British Summer Time event.
Robin Thicke headlined the Pepsi Max stage, which was also commandeered by Sean Paul and Clean Bandit.
The Boombox Stage, meanwhile, was headlined by 'La La La' hitmaker Naughty Boy.
Other celebrities who attended the third day of Wireless included Little Mix's Jesy Nelson, Frankie Sandford's soccer star fiancé Wayne Bridge, 'The Only Way is Essex' star Lauren Pope and actress Louisa Lytton.
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