This is the third time the band has taken home the top prize at the annual ceremony. "AM," the band's fifth studio album, sold more than 500,000 copies in the United Kingdom last year, the Brit Awards website said.
Arctic Monkeys also won the award for Best British Group Wednesday.
David Bowie was named Best British Male Solo Artist, while Ellie Goulding won the matching statuette for British Female Solo Artist.
New Zealand's Lorde scored the International Female Solo Artist honor, America's Bruno Mars won the International Male Solo Artist trophy and France's Daft Punk was declared Best International Group.
Rudimental and Ella Eyre's "Waiting All Night" earned the accolade for Best British Single.