The sophomore just knew he had to redeem himself, and his second-half recovery in several areas helped the sixth-ranked Orange rally for the 70-68 upset.
It was the second straight Saturday that No. 1 went down. Duke lost to then-No. 20 North Carolina State 84-76 a week ago.
A record crowd of 22,814 at the KFC Yum! Center saw Syracuse beat a No. 1 team for fourth time, all Big East teams.
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Carter-Williams' most important contributions were a go-ahead 3-pointer with 5:28 remaining, followed by a steal and go-ahead dunk with 23 seconds left as he scored nine of his team's final 11 points, including the last four.
He added a rebound and another steal at the end to cap a 16-point, seven-assist game that made it easy for Carter-Williams to forget a five-point first half and those two missed free throws.
"I wasn't going to go out without a fight," said Carter-Williams, who finished with four assists and four steals. "They were pressuring us, coming at us in the first half. Things were going their way. The second half, I tried to fight back the best I could. I had two or three turnovers but I just kept flipping the page, flipping the page and ended up winning the game, which was great. ...
"Those free throws, I just had to have faith in myself and just try to do anything to get the win."
Brandon Triche was 9 of 13 from the field, including five of Syracuse's seven 3-pointers, to finish with 23 points as the Orange (17-1, 5-0 Big East) took control of the Big East Conference. He credited Carter-Williams for getting the win.
"Michael was the reason we won the game, getting the dunk," Triche said. "I might have kept us in the game, but he's the reason we won the game getting the two steals. That's winning stuff."
Jerami Grant and C.J. Fair both had 10 points for the Orange, who won their seventh straight and beat the Cardinals for the third time in a row.
Russ Smith's 25 points led Louisville (16-2, 4-1), which had its 11-game winning streak stopped. The Cardinals shot 41 percent (24 of 59) including 29 percent in the second half.
After taking a 68-66 lead on Smith's two free throws with 1:58 remaining, Louisville missed two shots and committed two turnovers.
"That was a great college basketball game and they made some really terrific defensive plays down the stretch," Louisville coach Rick Pitino said. "They made the plays, they made the shots when it counted and we didn't."
Louisville's final chance to tie ended with a pass inside around Gorgui Dieng's knees in the final seconds which Syracuse recovered to seal the victory.
For the Cardinals, it was disappointing end to a week that began with their second No. 1 ranking in school history.
"I'd rather have the No. 1 ranking at the end of the year," Louisville guard Peyton Siva said. "I really don't mind having the No. 1 ranking at all. We're going to work our way back up to that spot and hopefully get it at the end of the year."
Syracuse was 24 of 49 from the field (49 percent) and the Orange outrebounded the Cardinals 36-31.
More impressive, Syracuse didn't wilt each time Louisville seemed to get the momentum in a back-and-forth game.
"I thought both teams played incredibly hard," Orange coach Jim Boeheim said. "There were opportunities where we could've gotten discouraged. Michael turned it over for a layup. He made some mistakes, but he is a big-time player.
"It was great, but now we can forget about it and try to get ready for Cincinnati on Monday night."
The game pitted Syracuse's trademark 2-3 zone defense against Louisville's signature pressure, which last year produced two games in which neither team shot above 35 percent in either game.
And while both teams got some results from their defensive strengths, the first half featured impressive offensive performances by both.
Syracuse made seven of its first nine shots and hit 14 of 23 overall (61 percent) thanks to Triche, who made all four 3-point attempts and all seven overall for 18 points by halftime. His accuracy helped put the Orange ahead early and then rally late in the half to forge a 38-all tie.
"I got comfortable," Triche said. "I didn't miss a shot in the first half. I was just letting the game come to me. I was going to get open spots and once I got open I just concentrated on following through. The guys got me the ball when I was open and it was pretty easy to move shots because of the movement we had. I wasn't going to force anything."
Louisville hit 54 percent (15 of 28) with huge contributions from its bench. Montrezl Harrell was a big factor in the Cardinals outscoring Syracuse's reserves 15-4, hitting all four of his shots for eight points one game after playing 4 scoreless minutes and being limited by an illness.
Smith led the way for the Cardinals' starters after a shaky start in which they missed their first three shots against the zone - including two from beyond the arc - before he hit a 3-pointer to bring Louisville within 6-3.
Syracuse quickly raised it to an 11-3 lead with help from Triche's first two baskets while his teammates added easy inside shots against Louisville's matchup zone. The Orange dominated on the boards as well with a 9-2 lead en route to 15-8 edge through 20 minutes.