The England captain had a nightmare night in north London as Spurs were dismantled with ease by Cristiano Ronaldo an co., giving the ball away on multiple occasions and generally proving to be ineffective in the final third.
And while Ole Gunnar Solskjaer will have enjoyed his evening, the same cannot be said for Nuno as fans turned on their boss, chanting 'You don't know what you're doing' and made their feelings clear at full-time with a loud chorus of boos.
The Portuguese seems like a man condemned and with the likes of Kane and Heung-min Son toothless in attack and unable to muster a shot on target during the 90 minutes, patience in the fanbase is already running out.
Spurs could have gone into the top four with a win, but that never looked on the cards and with five wins and five defeats from their opening 10 games, a challenge for Champions League qualification looks beyond this team.
And former Premier League striker Dean Ashton, who scored 17 goals in 44 Premier League appearances for Norwich from 2005-06, is convinced that the England captain doesn't want to be at the club and doesn't look happy under Nuno.
Asked how will Kane will be feeling whilst on commentary duty for talkSPORT, Ashton said: "I'd be feeling how he looks, which is despondent by his team's performance.
"He's a fantastic player but he still needs support, he still needs service, and he hasn't had any of that.
"He's not a miracle worker. But, also, he looks a mile off it.
"The few chances he did have tells you everything you need to know about Harry Kane, why is he not driving towards goal and striking the ball?
"A confident Harry Kane takes on chances like that on himself, he'll have that greedy look in his eyes and he'll only want to score.
"But today at times he's almost looking so early on, 'I want to pass this, I want to get rid of it', and that's so unlike Harry Kane."
Kane was booed in parts during the match for giving the ball away sloppily and Ashton admitted the striker looked 'disinterested' following the defeat.
"How often have you heard that, Harry Kane being booed?" he added.
"When forwards start to look disinterested, it's normally because - and I've been there - it's because you don't like what the manager is doing, you don't like the way the team's playing,, you don't like what you're doing in training.
"Too many times I looked at Kane and I looked at Heung-min Son and they didn't look happy.
"They didn't look like there was anything there for them. There was no idea, there wasn't a plan on how they were going to get back into the game. That's down to the manager.
"It was evident and very audible that the Tottenham fans were getting on top of the players, it wasn't just Nuno and Daniel Levy.
"But they've got to stick together now, because if they don't, if they start to break the group, it won't be long until Nuno's job will come to an end."