The Bayern Munich superstar found the net in the second leg of their last-16 victory over Bayer Leverkusen on Tuesday night.
Kane has already broken his own record from the 2023/24 campaign, when he found the net eight times during Bayern's run to the semi-finals.
This season's tally comes at an impressive pace - with the England captain racking up ten goals in just 11 games.
What's more, Kane could yet play another five Champions League matches this season if Bayern go all the way to the final.
The 31-year-old all-but sealed the German giants' place in the quarter-finals by opening the scoring at Leverkusen on Tuesday night.
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Having already netted twice in the 3-0 first-leg victory, Kane put the tie beyond the reigning Bundesliga champions with a well-taken goal in the 52nd minute of the return leg.
The Tottenham legend then turned provider for Alphonso Davies to make it 2-0 on the night and 5-0 on aggregate.
That assist made Kane the second Englishman in Champions League history to hit 50 goal contributions (39 goals, 11 assists) after David Beckham (16 goals, 36 assists).
Kane is looking to end his career-long trophy drought this season - with Bayern currently eight points clear of Leverkusen at the top of the Bundesliga table.
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The Englishman is also top of the goalscoring charts in Germany with 21 league goals in 23 games this season.
Kane broke a number of records in his debut campaign with the Bavarian club after an £82million move from Spurs in 2023.
Most goals by Englishmen in a single Champions League campaign
However, Bayern failed to win a single trophy, ending a run of 11 straight Bundesliga titles.
Kane is out for redemption in the Champions League having lost the final to Liverpool in 2019.
"To beat this team 5-0 [on aggregate] shows the type of team we are and the path we are on," said Kane.
"It's never easy to start with a 3-0 lead, but the intensity we showed, we had the better chances, we knew the game would open up in second half and we took our chances.
"We try not to listen to the noise too much, we know what we're capable of.
"This will only give us confidence performing against a top side."
Match Stats
Speaking about Kane breaking another record, manager Vincent Kompany piled praise on his striker.
He said: "It helps when you have a top player who wants to run and fight for the team like a youth player.
"I played against him as an opponent and he has become better with age. He has a way to work towards his performances.
"I trust his consistency and how he works towards his game and with that quality you always get your moments."
On the game in general, Kompany added: "These two wins, they don't decide the season but we have a lot of respect for Leverkusen.
"We did our work. "We did it well in the first 20 minutes and had the better chances.
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"Our aim was to win the first half and then to win the second half and we did that."
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Bayern will now face Inter Milan in the quarter-finals of the Champions League in April.
The Serie A leaders cruised to a 4-1 aggregate victory over Feyenoord on Tuesday to set up the mouth-watering tie.