After touching the ball the fewest times of any player in the first 45 or so minutes of an important game against Panama on Saturday (Sunday AEST) to wrap up group play, Kane needed one important header to make history.
In the 67th minute, he scored his 11th career World Cup goal to break a tie with Gary Lineker for the country's most on soccer's biggest stage.
"It's fantastic that he has the chance to break this record in a World Cup when it really matters," coach Thomas Tuchel said after England beat Panama 2-0 to win their group.
"Everyone's very happy for Harry because he's a fantastic teammate. That makes it very special. He's loved by everyone, respected by everyone."
Jude Bellingham, who scored a few minutes earlier to relieve some of the tension building up on the field and in the stands full of red-and-white clad fans, made the pass to Kane, who outjumped Andres Andrade and headed a ball past diving goalkeeper Orlando Mosquera.
"Jude with a great bit of play and a great cross," Kane said. "He kind of just hung it up, and I was kind of waiting for that one throughout the game — just to get across my man there — and it was nice to see it go in."
This particular goal was the result of the chemistry Bellingham and Kane built up over several years playing together.
"It's quite easy to play with him," Bellingham said.
"He's at a level at the minute that's just incredible. You don't doubt him at all in terms of whether he's involved, whether he's not. You know he's going to make a difference in the game, and he did again."
There did seem to be doubt at halftime, when Kane was a non-factor with 10 touches and England were never close to scoring. Down the road in Philadelphia, Croatia's lead on Ghana turned up the pressure.
But there was far more jump out of halftime, and the soon-to-be 33-year-old striker was a big part of the improvement on the way to a victory that looked on the scoreboard more convincing than it felt for much of the time it was being played.
The goal was Kane's 82nd playing for England internationally, adding to his own record. Teammate Jordan Henderson, now at his fourth World Cup, recalled Kane scoring twice in the opener against Croatia to match Lineker and mistakenly thought this mark was already in Kane's sole possession.
"It seems with age, he's just continued," Henderson said. "He's smashing records everywhere he goes and scores so many goals. He's been an incredible player so far for England and continues. He's still got a long way to go.
"But, yeah, he deserves everything he gets. He's been an incredible player, an incredible teammate and delighted for him to be able to get that record."
Bellingham considers Kane England's best player of all time, "the one who's showed up more than anyone, more than any England player."
Kane even scored with another icon, David Beckham, watching from the stands with his face flashed on video screens to massive cheers.
"Obviously another proud one to reach, for sure, No. 11," said Kane, who now has three goals this tournament. "I hope it's not the last this tournament."
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