The 24-year-old Matthews scored a hat trick against the host Tampa Bay Lightning in the Maple Leafs' 6-2 victory to pull even with Vaive, whose record has stood for over 40 years (1981-82 campaign, which also was the highest-scoring season in modern NHL history).
"It's humbling, it means a lot,'' Matthews told reporters postgame.
Matthews previously joined the Leafs' elite group of 50-goal scorers when he hit the mark against Winnipeg on Thursday. In Toronto's 104-year history, only three players before Matthews had ever notched 50: Vaive (three times in the 1980s), Gary Leeman (1990) and Dave Andreychuk (1994).
Perhaps most impressively, Matthews needed just 63 games to score his 54th goal. He had already recorded the fastest 50-goal season since 1995-96. The last player to hit 50 at the same point in his season as Matthews did this year was Alex Ovechkin in 2007-08. And on the road to 50, Matthews was scoring at a blistering pace that included at least one goal in 31 of 45 games leading up to the feat.
Now he's on track to set an entirely new franchise-best in Toronto, one he could continue building on this season and maybe surpass in ones to come. Matthews also moved past Bob Pulford into ninth place on Toronto's all-time goal list with 253 career goals.
"It's fun to watch him,'' Maple Leafs goalie Jack Campbell said of Matthews. "To see him get the results on the ice like he's been doing, it's just incredible. It's just crazy. It's amazing."
Matthews won his franchise's first Rocket Richard Trophy (NHL's leading goalscorer) in last year's COVID-19 shortened campaign, on the strength of a 41-goal showing in 52 games. He previously scored 47 goals in 70 games the year before.
He's been battling Edmonton's Leon Draisaitl to secure a second consecutive Rocket title. As Matthews sits at 54 goals, Draisaitl is behind him with 50.
The Maple Leafs took a two-point lead over Tampa Bay and Boston for second place in the Atlantic Division with Monday's win.
"This is a big game for us, obviously," Matthews, said. "They're a really good team, they know how to win, so it was an important game for us this point of the season. All these points count and really matter. I think it's just a really complete game by everybody.''
The Associated Press contributed to this story.