The 'Live While We're Young' group were up against Muse, Mumford & Sons, Alt-J, Justin Bieber and Ed Sheeran in the category, and were revealed as the 'winners' at a ceremony hosted by Russell Kane at London's Troxy on Wednesday night.
It is the second year in a row that the group have picked up the unwanted title.
Meanwhile, Styles 'beat' Skrillex, Psy, Fred Macpherson, Azealia Banks and David Cameron to the dubious 'Villain' honour, while last year's recipient Bieber failed to make the nominations.
Styles previously quipped that he wanted to win the award, noting: "You've got to take the rough with the smooth but I don't really feel like I've done anything that bad. Should be fun!"
After his award was announced, Styles wrote on Twitter: "And thank you to @NME for my award tonight. Gotta take the rough with the smooth eh?"
Jake Bugg, who criticised the boyband earlier this month, told reporters at the ceremony: "I don't know how they can really be considered a band, to be honest. They're there to look good. Music wise? I assume they don't really have a clue.
"We'll just see. They might do. Probably the ugliest one is the best singer. He might know a couple of chords."
Elsewhere at this year's NME Awards, Florence Welch and The Rolling Stones took home two gongs apiece, while there were also accolades for Biffy Clyro, Arctic Monkeys and The Killers.
> Read the full list of winners at this year's NME Awards
Photo gallery - NME Awards 2013 red carpet:
Copyright: PA Images Jonathan Brady/PA Wire