Former Chelsea and Manchester United boss Mourinho has signed a contract until the end of the 2022-23 season.
"The quality in both the squad and the academy excites me," said the 56-year-old Portuguese. "Working with these players is what has attracted me."
Spurs chairman Daniel Levy said: "In Jose we have one of the most successful managers in football."
Tottenham reached the Champions League final last season under Pochettino, but lost 2-0 to Liverpool in Madrid.
The Argentine, who was appointed in May 2014, did not win a trophy in his time in charge of the north London club, with Spurs' last silverware being the League Cup in 2008.
Levy added: "He [Mourinho] has a wealth of experience, can inspire teams and is a great tactician.
"He has won honours at every club he has coached. We believe he will bring energy and belief to the dressing room."
Mourinho still has a home in London and won three Premier League titles - in 2005, 2006 and 2015 - as well as one FA Cup in two spells at Chelsea.
Having taken over at Manchester United in May 2016, he won the Europa League and Carabao Cup with them in 2017.
Mourinho was sacked by the Old Trafford club in December 2018, with the club 19 points behind league leaders Liverpool at the time, and had not managed another side before joining Spurs.
He has also previously managed Portuguese side Porto, where he won the Champions League in 2004.
At Italian club Inter Milan, Mourinho won a league, cup and Champions League treble in 2010 and was named Fifa's world coach of the year, while he led Spanish team Real Madrid to the La Liga title in 2012.
He takes over a Spurs side that are without a win in their past five games and have slipped to 14th in the Premier League, 20 points behind leaders Liverpool after just 12 matches.
The Portuguese's first match in charge is a trip to West Ham United on Saturday (12:30 GMT kick-off).
Mourinho has turned down a number of managerial opportunities, including in China, Spain and Portugal, since leaving Old Trafford.
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