The Spurs superstar has recently been linked with a move to Bayern Munich, but has clearly not let that affect him as he fired in a double during his side's trip to Scotland.
New Rangers signing Antonio Colak opened the scoring for the hosts, after good work by fellow summer addition Rabbi Matondo.
But Kane soon sparked into life, firstly scoring with a trademark whip into the far corner, before teammate Heung-min Son teed him up for a second, as was so often seen last season.
The victory saw captain Hugo Lloris lift the Walter Tull Memorial Cup, which was first awarded when the two sides last met during a pre-season friendly in 2004.
The trophy was awarded in memory of Britain's iconic first black outfield player who had links to both clubs during a playing career cut short by his death during World War I.
On social media, a selection of rival fans joked that Spurs have now finally ended their 14-year trophy drought.
Of course, this wasn't the case, with trophies in pre-season friendlies not recorded in official records.
Despite failing to win any major honours since their 2008 League Cup triumph, the north Londoners' pre-seasons have been trophy-ladened in comparison.
Spurs won the International Champions Cup in 2018 and the Audi Cup a year later.
And boss Antonio Conte says he is 'very happy' after the win, as his side prepares for their Premier League opener against Southampton in two weeks' time.
"I'm happy because the game wasn't a friendly game, it was a real game," Conte said after the game.
"You know very well that the last game they played against West Ham they won 3-1 and the fitness of Rangers is higher, in front of us but, despite this, I think that we played with good intensity, good pressure and good quality.
"If I have to find a situation that today was to improve it was because we created a lot of chances, especially in the first half and we didn't score, but I understand we are still improving and are also a bit tired because the pre-season is also important for us to make the fitness at the high level.
"But I'm happy because I repeat the tactical aspect I'm very pleased. For sure we can improve because we conceded a goal that we can avoid, but I'm delighted with the attitude and the will and desire that the players are showing me in this pre-season. I'm very happy."