The England captain drew level with Greaves on 266 goals for the north London club when he fired in the opening goal against Fulham at Craven Cottage on January 23.
But Kane’s winner against the reigning Premier League champions put him ahead of Greaves as the standalone record holder on 267 strikes, and brought up his double-century in the English top flight in the process.
'A GOAT in this league' - Kane hailed by stand-in Spurs boss Stellini after landmark goal
Talking afterwards to Sky Sports, Kane said: “It’s hard to put into words and I’m so glad it [the record-breaking goal] came in a win.
“We worked so hard to keep a clean sheet. It was so special to do it in front of the fans. There has been so much talk about it in the last couple of weeks and to do it in such a big game is even more special.
“It is a great feeling. When I started playing regularly it wasn’t even in my imagination to score 200 Premier League goals and I have a few more years left so hopefully there are more to come.
“[Jimmy Greaves] is a complete hero, one of the best strikers to play the game so to be in that conversation is special. And to overtake him is a huge moment for me.”
Greaves’ record had stood since 1970, when the striker joined West Ham to end a nine-year spell at Spurs in which he scored 266 goals in 379 games.
Kane needed 415 games to reach the same tally but has now usurped the England World Cup winner.
Greaves won two FA Cups and the Cup Winners’ Cup during his time at Spurs, but Kane is still looking for his first piece of major silverware in his 13th season at the club.
Kane has picked up several prestigious individual awards, winning the Premier League Golden Boot three times and the World Cup Golden Boot in 2018.
The 29-year-old is also third in the all-time Premier League goalscorer standings, behind Wayne Rooney on 208 goals and Alan Shearer on 260 goals.
Harry Kane of Tottenham Hotspur celebrates after scoring the team's first goal. Kane scored his 267th goal and overtakes the late Jimmy Greaves to become the Spurs’ all-time leading scorerHarry Kane of Tottenham Hotspur celebrates after scoring the team's first goal. Kane scored his 267th goal and overtakes the late Jimmy Greaves to become the Spurs’ all-time leading scorer

Harry Kane of Tottenham Hotspur celebrates after scoring the team’s first goal. Kane scored his 267th goal and overtakes the late Jimmy Greaves to become the Spurs’ all-time leading scorer

Image credit: Getty Images

Kane has been in fine form for Antonio Conte’s side this season, with his record in the league now standing at 17 goals from 22 appearances.