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Sammy Zeglinski hit 5-of-8 from behind the arc in route to a 19-point effort for the Cavaliers (13-6, 4-2 ACC), who were coming off consecutive losses, including an overtime setback to Virginia Tech on Thursday.
Will Graves and Larry Drew paced the Tar Heels (13-8, 2-4) with 15 points apiece.
The reigning NCAA champions have now lost four of their last five, the only win in that span coming against conference bottom-dweller NC State on Tuesday.
Virginia led 35-30 at the break and rattled off 18 consecutive points following an Ed Davis bucket to open the second half scoring.
Zeglinski hit a pair of three-pointer during the critical run, which Jerome Meyinsse capped with a old-fashioned three-point play for a commanding 53-32 cushion with just over 14 minutes left.
The margin was double digits the rest of the way.