Codi Miller-McIntyre added 12 points for the Demon Deacons (11-3, 1-0), who took control with a 15-2 run midway through the second half to build a double-digit lead.
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The Tar Heels (10-4, 0-1) made a late push to cut the deficit to 64-61 with about 2 minutes left, but got no closer as the Demon Deacons held on for their third win against a ranked opponent under fourth-year coach Jeff Bzdelik.
The win also snapped a four-game losing streak in the long-running series, giving Wake Forest its first win against North Carolina since 2010.
James Michael McAdoo had 13 points and eight rebounds to lead the Tar Heels, while J.P. Tokoto and Brice Johnson both added 12 points and nine rebounds.
