The England international, 23, is one of the most potent marksmen in the Premier League, but until Sunday none of his 70 goals had been at the expense of the Red Devils.
The hoodoo was ended, however, after 512 minutes of frustration as he sent Spurs 2-0 up by converting Christian Erikson's cross.
Kane brought his Premier League tally to 71 goals with the strike, a mark he has reached in just 110 games.
With 22 goals in the 2016-17 league season alone, the star has been one of the main reasons Spurs pushed Chelsea to the final games of the season in the title race.
And with his goal to put the hosts further ahead of United, he also managed an additional distinction.
1 - Harry Kane has now scored against 24 of the 25 opponents he has faced in the Premier League (Cardiff being the exception). Portfolio.— OptaJoe (@OptaJoe) 14 de mayo de 2017
The striker has now scored against 24 of the 25 Premier League opponents he has faced, with only Cardiff escaping his wrath in front of goal.