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Kimbra, with Gotye, won in the 'Record of the year' and 'Best pop duo' categories at the 55th Grammy Awards in Los Angeles.
She was presented with the 'Record of the year' award by Prince.
However, Flight of the Conchords star Bret McKenzie lost out on the award for best song written for visual media at the star-studded awards in Los Angeles.
The win is massive achievement for the New Zealand songbird and caps off the huge success from her album Vows last year.
Meanwhile, McKenzie's song Man or Muppet lost out to Safe and Sound by T-Bone Burnett and Taylor Swift in the best song written for visual media category.
Safe and Sound was on the soundtrack for the hit film The Hunger Games.
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Man or Muppet took best song at last year's Oscars.
Hamilton-born Kimbra returned to Los Angeles last week for the premiere music awards ceremony, which started at midday.
The 22-year-old has been posting online of her excitement at seeing pop singer Justin Timberlake, rocker Jack White and hip-hopper Frank Ocean perform at the Grammys.
"The day of the Razzle Dazzle begins," Kimbra posted on her Twitter account this morning.
"Prince will be at [the Grammys] presenting an award tonight. Breathe, breathe," she said.
News.com.au reports that Spotify's analysis of the most popular Grammy-nominated artists puts Somebody That I Used To Know as the best placed to win Record Of The Year.
The same data also suggests Australian Gotye and Kimbra will win best duo for their duet.
However, the awards are not publicly voted so the choices of music fans are unlikely to sway industry opinion, Spotify has warned.
Australian betting agency sportsbet.com.au also has the duo's hit as a favourite for Record Of The Year, paying $2.10 for the win.