Indie pop band fun. won best song Grammy for "We Are Young," one of six categories in which they were nominated at music's biggest awards show.
The New York group are also shortlisted for the three other top categories of best record, best album and best new artist, as well as best pop vocal album and best pop duo/group performance.
Their beaten rivals in the best song category were Ed Sheeran for "The A Team," Miguel for "Adorn," Carly Rae Jepsen for "Call Me Maybe" and the songwriters of Kelly Clarkson's "Stronger (What Doesn't Kill You)."
The band topped Grammy nominations announced in December.
If they were to win all four of the major categories, it would mark the first such achievement in more than 30 years, according to The New York Times.
British songstress Adele won the Grammy for best pop solo performance, the first award handed out during the main event.
She also gave a typically straight-talking answer when asked how she is feeling about the Oscars later this month, where she is nominated for best song for the theme tune to Bond movie "Skyfall," admitting she was nervous.
The 24-year-old singer, who swept the board with six Grammys at last year's awards show, took the pop performance prize for a live rendition of her hit "Set Fire to the Rain."
"My good luck charm, J-Lo," she said as she accepted the award from Jennifer Lopez and Pitbull. "This is amazing. I wanted to come and be part of the night. I loved it last year, obviously," she added.
Last year she won best song, best record, best album for her breakthrough "21," best short video, best pop album and best pop artist, winning all six categories in which she was nominated.
Speaking backstage after accepting her award Sunday, Adele said it was less stressful this year than last, even though she is now a mother, having given birth in October.
"I've been up since 6:00 am so I'm quite tired," she told reporters, but added that, as a new mother "it's nice, I haven't been as stressed out... you have to prioritize what you stress about and worry about."