After Pierre-Emile Hojbjerg done an outstanding job of finding Kane inside the area, the England captain surpassed the milestone with a cool finish from 10 yards out.
Fans sprang from their seats to clap for the 29-year-old striker, who scored his first goal for Spurs on December 15, 2011, when a message reading “Congratulations Harry Kane” lit up on the scoreboard inside the stadium.
Kane scored his 200th goal in the Premier League in the 15th minute; only Wayne Rooney (208) and Alan Shearer (260 goals) have scored more.
It happened unexpectedly and while Tottenham manager Antonio Conte was recuperating at home following gallbladder surgery.
Tottenham, who played the final few minutes with 10 men after defender Cristian Romero was dismissed for
Kane, who was 18 when he scored his first goal for Spurs against Shamrock Rovers in the Europa League 12 years ago, celebrated his historic goal with all the vigor of a young man.
It seemed appropriate that it occurred at the Tottenham Hotspur Stadium in front of his team’s supporters, who erupted into a raucous cheer after the ball sailed past City goalkeeper Ederson.
Greaves scored 266 goals after 379 games, compared to Kane’s 267 goals in 416 games.
The only letdown was that his manager Conte was not in the stadium to see the goal.
After his procedure, the Italian was absent, and Cristian Stellini, his assistant, took over against City.
After the goal, Kane’s teammates and the Tottenham coaching staff remained on the field.