Carolina erased an early one-goal deficit by dominating the second period, in which they outshot the host Maple Leafs 20-5 and got goals from Eric Staal and younger brother Jordan.
"Eric had a big goal to get us up and going again and he's been the star for us this year and it was nice for me to chip in as well," Jordan, 24, who was traded to Carolina from Pittsburgh last June, told reporters. "Hopefully there will be many more of those nights for us."
The Hurricanes (4-4) tied the game 81 seconds into the middle frame when Jordan, who was left alone in front of the Toronto net, received a pass from Patrick Dwyer and coolly deked goalie James Reimer for his first goal of the season.
Carolina captain Eric Staal, 28, scored what proved to be the game-winning goal when his pass from the side of the net deflected off a Toronto defender and into the Maple Leafs net midway through the second period.
It marked the first time in 27 years that brothers scored in the same game for the Hurricanes franchise, which was based in Hartford, Connecticut, when Dave and Wayne Babych accomplished the feat in 1986.
Third period tallies from Justin Faulk, who scored on a two-man advantage 43 seconds into the final frame, and Dwyer put the game out of reach for Toronto, who dropped to 1-4 at home.
The loss extended Toronto's worst start on home ice since dropping the first six home games in the 2009-10 season. It also proved dispiriting for the Maple Leafs fans as chants of "Let's go Blue Jays" rang through the packed arena in a show of support for the city's revamped Major League Baseball club.
Ward allowed the opening goal less than six minutes into the game when Matt Frattin shoved a rebound by him, but the former Stanley Cup-winning goalie was brilliant the rest of the way and turned aside 41 of 42 Toronto shots in total, including several chances from in close.
The Leafs (4-5) thought they had tied the game late in the second period but after a lengthy review, the referee ruled that Tyler Bozak had kicked the puck in the net.
"It took a little bit to get our legs," Ward, whose 41-save performance was his highest total of the season, told reporters.
"But we really took over in the second period, got our feet moving, capitalized one some opportunities and got the momentum."
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