Djibril Sidibe racked up an nearly similar close-range objective on 43 mins, and Kane added his second from the place (48) as Raphael Varane saw red for a last-man foul on Dele Alli.
England have also lost to Germany and drawn against Spain this season.
Before the game, a touching tribute to the victims of the Manchester and London terror attacks saw a rendition of "Don't Look Back In Anger" and a minute's silence.
When attention turned to football, those in attendance bore witness to a superb team goal inside just nine minutes as England clicked in style. Dele Alli's fine cross-field pass picked out Raheem Sterling, who brought the ball under control before back-heeling to Ryan Bertrand.
France were quicker, more aggressive and more youthful.
France were swift to respond with Olivier Giroud hitting the net with a lovely volley ruled out for offside before Dembele blazed wide.
England did not heed those warnings and France pulled level midway through the half, despite seeing full-back Benjamin Mendy limp out of the action. Giroud was allowed to meet a free kick with a powerful header that Tom Heaton did well to stop. But the Burnley goalkeeper, making his first start, could not stop Umtiti rifling home the loose ball.
After sparing England's blushes against Scotland, Harry Kane was in the right place again to give England the lead against France. We have got to find a way to win that - we just weren't good enough.
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France capitalised on England's fragile defence two minutes before half-time.
Dembele left John Stones for dead inside the penalty area before seeing his effort saved by Heaton, but once again the ball bounced out into a unsafe area and this time Sidibe was there to stroke home the rebound and send France into the break ahead.
HARRY KANE scored twice last night but England crashed to a sloppy defeat against ten-man France.
England were second best against a young, confident French side. But I think we've had to play at our absolute limit to stay in all three of the matches, which has shown in the latter stages of those games.
"In the space of 90 minutes we saw what we're very good at".
With France down to ten men England should have taken the initiative, but it was a sloppy ball from Gary Cahill which let Les Bleus in once again, allowing Ousmane Dembele to bag his first goal at worldwide level, which turned out to be the victor. He tries to move the ball outside, Bertrand puts is back into his stride, and he speeds into the box, feints outside, ducks inside as Stones goes shopping, and shoots low and hard.
"We've just got to learn quickly how to manage games in situations like that. Their pace and their athleticism were a problem for us".
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