Tottenham's ambitions of finishing in the top five took a huge dent after a 3-1 defeat to Sheffield United.
Goals from Sander Berge, Lys Mousset and Oli McBurnie sealed a deserved three points for Chris Wilder's side, who bounced back from their own poor recent performances.
Spurs boss Jose Mourinho had been hoping to build on last week's 2-0 victory over West Ham, but his team were outfought in all departments by the Blades.
Wilder's side took the lead in the first half thanks to a Sander Berge goal, but the visitors thought they levelled the scores through Kane after the England striker curled past Dean Henderson.
However, the goal was ruled out after VAR ruled that Lucas Moura handled the ball in the build-up.
The hosts doubled their lead in the second half thank to substitute Mousset after good work from Enda Stevens, before McBurnie all but sealed the win with six minutes to go.
Kane did get his goal, tapping in from a Son Heung-min cross, but it proved to be nothing but a consolation for Spurs.
After the match, rival supporters took to social media to mock Tottenham, with the north London side now outsiders to get European football.
The result leaves Spurs ninth in the table, a point behind rivals Arsenal and nine behind fourth placed Chelsea.
Tottenham next face Everton at home on Sunday, before travelling to struggling Bournemouth next Thursday.
Mourinho's side then host Arsenal in the north London derby three days later.
