Myles Powell added 19 points and Angel Delgado scored 13 for the Pirates (22-11), who led the entire way a year after a late meltdown cost them an early exit against Arkansas.
Seton Hall will play top-seeded Kansas on Saturday in the second round of the Midwest Regional.
Allerik Freeman hit six 3-pointers and had a career-high 36 points to lead the No. 9 seed Wolfpack (21-12), who returned to the tournament under first-year coach Kevin Keatts for the first time in three years. Torin Dorn added 18 points and 12 rebounds, and Lennard Freeman contributed 13 points.
The only thing that slowed down the high-scoring, up-and-down matchup was the whistles. The teams combined for 53 fouls, resulting in 66 total free throws. Seton Hall had two players foul out - Delgado was one of them - and the Wolfpack had three players relegated to the bench.
"We just couldn't stop them, said Lennard Freeman. "We couldn't get complete stops."
For both Freemans, the loss meant the end of their college careers.
"It was win or my college career is over, so every bit of what I was doing out there was just because I didn't want to go home," said Allerick Freeman.
Three other players finished the game with four fouls apiece.
"There were a lot of whistles," Dorn said, "but coach always preaches you have to win all types of games. We just weren't able to do that."
The high-scoring tempo was set early on, when the Pirates scored on their first eight possessions and hardly missed a shot. If not for Allerik Freeman's outside shooting, the bruising boys from the Big East might have put away their stunned ACC rivals before halftime.
The Wolfpack made a run of its own midway through the half, but was never able to gain the lead, and Seton Hall used another late charge to take a 51-41 lead into the locker room.
Lots to be proud of if you're a Wolfpack fan. It seems like they ran out of gas losing 3 of their last four games.— Joe Mazur (@joemazurabc11) March 15, 2018
North Carolina State closed within 63-60 midway through the second half, as Freeman began to complement his 3-point shooting by slashing to the basket for easy layups. But he didn't get a whole lot of help from a team that had relied on balanced scoring all season.
During one five-minute stretch, Freeman was the only one wearing red to score.
Carrington and Powell were just effective at the other end for Seton Hall. They combined to score 12 straight points for the Pirates, highlighted by a 10-2 run to seize control, and the starting guards showed plenty of poise when North Carolina State tried to make one last run.
North Carolina State hung tough thanks to Freeman, a transfer from Baylor, who went 6 of 8 from beyond the arc. But the rest of the Wolfpack were just 5 of 22 from 3-point range.
Seton Hall only committed seven turnovers, won the rebounding battle and took advantage of North Carolina State's foul trouble. The Pirates went 31 of 39 from the foul line.
The Pirates advanced to play the Jayhawks, a 76-70 winner over Pennsylvania, in the second round on Saturday, while the Wolfpack resume Keatts' building job as he looks toward Year 2.