Kane pounced to finish at the back post following Mousa Dembele's flick from a corner early in the second half.
He then rose to head home in the 86th minute to take Spurs above the Gunners in the Premier League table.
Mesut Ozil had given Arsenal the lead with a close-range finish but they sat back after and paid the price.
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Spurs have now won their last seven home matches and taken 22 points from a possible 27.
They also have a very real chance of ending a run of 18 seasons in which they have finished below Arsenal in the Premier League table.
And they have a superstar in the shape of Kane, who now has 22 goals for the season, four in his last two games, and must surely have done enough in front of watching Roy Hodgson to warrant a call-up to his England squad.
Twice in the second half he breached an Arsenal backline that had previously looked as stubborn and solid as it had during last month's impressive 2-0 win at champions Manchester City.
His first goal was an opportunist strike, arriving at the back post to finish after Dembele's flick-on from a corner.
His second was a headed finish of the highest quality as he rose above the Gunners defence and guided his effort past the flailing David Ospina.
He could have been on the scoresheet sooner but his long-range shot was well saved by Ospina during a first half in which Spurs were the more positive side, but ended it behind when Olivier Giroud's fluffed finish from Danny Welbeck's cross fell to Ozil to finish from inside the box.
At the break, Arsenal were eyeing another efficient counter-attacking victory in the mould of their Etihad triumph - a win that would have been their 13th in 16 games.
Wenger's side had chances in the second half - most notably a long-range Welbeck shot that was well saved by Hugo Lloris - but in general they were not at their best as they became the latest side to suffer at the hands of Spurs and their in-form striker.
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