And Spurs fans showed their appreciation for the 30-year-old by chanting for him to stay as links with a move to Bayern Munich continue.
In their penultimate pre-season friendly of the summer, the north London side hosted Shakhtar Donetsk to raise funds for the humanitarian crisis in Ukraine as a result of Russia's invasion.
Kane was named captain in a strong starting XI by Ange Postecoglou as they work their way towards the new season.
With seven minutes remaining in the first half, the club's all-time record goal scorer netted from the spot to give them the lead.
Shakhtar equalised on the stroke of half-time through Kevin Kelsey, but Kane restored Spurs' lead at the start of the second half.
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Summer signing James Maddison was the provider in a combination that fans will be hoping to watch week in, week out this season.
Kane then scored his third of the afternoon before the hour mark after Dejan Kulusevski's through ball.
Fans at the Tottenham Hotspur Stadium could be heard singing 'Harry Kane, we want you to stay' as their star man put in another excellent performance.
He netted his fourth in the 79th minute, this time tapping home after Manor Solomon's shot was saved and fell into his path before he was substituted to a standing ovation.
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And his replacement Dane Scarlett made it 5-1 with the last kick of the game for Spurs.
However, the England captain could be heading out of London this summer and opt for a switch to Munich.
Bayern have sent Spurs an £86million take it or leave it offer for the striker, whose contract expires next summer.
Reports earlier in the week claimed that the Bundesliga champions had given a deadline of midnight on Friday to respond.
However, Spurs chairman Daniel Levy seems to have ignored such a demand and has flown to Miami on holiday with his family instead.
talkSPORT understands that Kane himself is not actively trying to force a move away from the club.
However, should Spurs not agree to sell him this summer, they would may lose him for free in 2024.
Despite the speculation that has been hanging over his head for some time, Kane is continuing to prove his immense quality in front of goal.