Neal opened the shootout by beating James Reimer before Crosby sealed the victory by scoring on Pittsburgh's second attempt after Marc-
Andre Fleury stopped Toronto's Tyler Bozak and Nazem Kadri.
Toronto's Phil Kessel forced overtime with his seventh of the season at 15:40 of the third before an Air Canada Centre gathering of 19,418.
Neal, Crosby, Beau Bennett and Pascal Dupuis scored in regulation for Pittsburgh (17-8-0), which outshot Toronto 41-26. Crosby scored in his first game at the ACC in over three years to extend his points streak to a season-high seven games (five goals, 10 assists).
James van Riemsdyk, Cody Franson and Clarke MacArthur had the other goals for Toronto (15-10-1) while captain Dion Phaneuf added three assists.
Crosby, the Penguins' captain who leads the NHL in scoring with 40 points (12 goals, 28 assists) skated at the ACC for the first time since Jan. 9, 2010. In 11 career visits here, Crosby has 15 points (nine goals, six assists) and extended his points streak versus Toronto to eight games.
Then again, the 25-year-old from Cole Harbour, N.S., has excelled against Toronto, having registered 38 points (19 goals, 19 assists) in 24 career games.
Pittsburgh outshot Toronto 13-5 in the first and wasted little time opening the scoring as Neal registered 16th of the season just 36 seconds in. Matt Niskanen's point shot was partially blocked but the puck dribbled into the slot, where Neal fired a shot past James Reimer.
Van Riemsdyk tied it at 7:14 on the power play with his 14th goal but Crosby and Bennett combined to give Pittsburgh a 3-1 lead. Crosby registered his 12th goal at 14:31 after Reimer couldn't control Kris Letang's shot, allowing Letang to get the rebound back to Crosby. Bennett's shot got past Reimer at 15:21, giving Bennett his second of the season.
Franson's second of the year pulled Toronto to within one on the power play at 10:12 of the second with Crosby off for tripping. Dupuis put Pittsburgh ahead 4-2 at 13:01 with his ninth but MacArthur made it 4-3 a minute later with his seventh.
Reimer finished with 37 saves on 41 shots.
NOTES -- Forward Matt Frattin returned to Toronto's lineup after missing 12 games with a knee injury . . . Pittsburgh's Evgeni Malkin drew an assist on Bennett's goal, giving him points in nine of 11 career visits to the ACC . . . Toronto came into Saturday's game leading the NHL in hits (773) and fighting majors (25) . . . The Penguins return to the ACC to face the Leafs on Thursday night . . . Crosby entered action Saturday averaging 1.63 points per game, the NHL's best mark since Penguins owner Mario Lemieux (1.77 points per game) in 2000-'01.
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