John Hugley scored 18 points, Jamarius Burton added 14 points and seven rebounds, Mouhamadou Gueye had 11 points and Femi Odukale 10 for the Panthers (11-16, 6-10 ACC), who won their third straight conference game for the first time since 2014.
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Caleb Love scored 15 of his 19 points in the final 5:11 for the Tar Heels, who trailed 40-23 at the half.
Brady Manek added 12 points and 10 rebounds and Kerwin Walton and Leaky Black had 11 points each.
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Leading scorer and rebounder Armando Bacot picked up his fourth foul with eight minutes to go and remained on the bench finishing with seven points and eight rebounds.
In the Tar Heels' previous game, UNC (18-8, 10-5 ACC) outscored Florida State 62-24 in the first half of a 20-point win. But Wednesday, it was the Panthers taking off to a huge lead after shooting 60%, over 30% better than UNC in the first half.
When Bacot - who leads the ACC with 19 double-doubles this season - picked up his fourth foul, the Tar Heels were trailing by 19. They rallied without him as Love scored 13 straight UNC points and assisted a Manek basket to pull within 69-63 with 1:50 to go. But they wouldn't get closer with Hugley scoring five points down the stretch.
Pitt finished at 51% shooting, including 10 of 17 from the arc. UNC shot 41%, 7 of 26 from 3-point range.
Pitt beat UNC for the third time in their last four meetings and won for the second straight time at Chapel Hill.
Pitt is home against Georgia Tech on Saturday. UNC is at Virginia Tech on Saturday.