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Mourinho was brought in to take the club to the next level and win trophies following Mauricio Pochettino’s sacking in late 2019, but Spurs currently sit seventh in the Premier League and are out of every cup competition bar the Carabao Cup.
Following the 2-2 draw at Everton on Friday night, chairman Daniel Levy informed the former Manchester United manager of his decision on Monday morning - the morning after the stunning news that Spurs are one of the 12 founding members of a new European Super League.
Tottenham have won just one of their last five in the Premier League and in that time were knocked out of the Europa League by Dinamo Zagreb.
In a statement, Levy said: “Jose and his coaching staff have been with us through some of our most challenging times as a club. Jose is a true professional who showed enormous resilience during the pandemic.
“On a personal level I have enjoyed working with him and regret that things have not worked out as we both had envisaged. He will always be welcome here and we should like to thank him and his coaching staff for their contribution.”
Mourinho's coaching staff of Joao Sacramento, Nuno Santos, Carlos Lalin and Giovanni Cerra, have all left with immediate effect.
The Portuguese has divided the dressing room in recent weeks, regularly taking aim at his players after disappointing results.
Ryan Mason and Chris Powell will take temporary charge of the side, with Tottenham facing Southampton on Wednesday before the Wembley final against Pep Guardiola’s side on Sunday.
RB Leipzig manager Julian Nagelsmann is an early favourite to succeed Mourinho at the Tottenham Hotspur Stadium, along with Leicester manager Brendan Rodgers.
Mourinho signed a deal until 2023 when he replaced Pochettino and took Spurs from 14th in the Premier League to sixth in his first season.
Tottenham were top of the table earlier this season but form took a nosedive and he leaves with the north Londoners five points behind West Ham in the final Champions League place.
The 58-year-old’s sacking means Tottenham become the first club that Mourinho has not won any silverware with.
The former Chelsea and Real Madrid boss has become increasingly sour during dealings with the media in recent weeks. After Standard Sport reported that Mourinho's claims over Toby Alderweireld returning late from international duty were false, he accused the media of playing games, while his comments after a draw at Newcastle were not well received by certain members of the squad.
Mourinho accused his players of not being up to the level of the Premier League, telling the BBC: "The Premier League is hard and is high-level football. And when in some actions you don't show that you belong to that high level of football, it's difficult."
When it was put to Mourinho that he was famous for holding onto a lead, he said: "Same coach, different players."
Mourinho was asked last week why his side had dropped 18 points from winning positions this season, and he said he knew why but may never reveal it.
After years of entertaining and attractive football under Pochettino, Mourinho's more pragmatic and negative style - meant to improve results - has angered supporters with many turning on the manager in recent weeks and some having never come to terms with the appointment.
It is thought Levy's decision could see the club have to pay out tens of millions in compensation to Mourinho.