Benfica said on Thursday that they had reached a deal with Mourinho, sealing his return to the country 21 years since he led their deadly Portuguese rivals Porto to the Champions League title in 2004.
The coach was officially introduced in a news conference, and later in the day was set to oversee the squad in a practice session.
"Being Portuguese, it's obvious that everyone knows well the history and the dimension of this club," Mourinho said.
"I'm now the coach of one of the greatest clubs in the world. None of the other giant clubs that I coached in the world made me feel so honoured and motivated as I am now as the coach of Benfica."
Mourinho started his coaching career at Benfica in 2000 but lasted only three months before leaving in a contract dispute.
He will be back in the Champions League after a five-year absence, since a round-of-16 exit while coaching Tottenham in 2020. Mourinho also won the Champions League with Inter Milan in 2010.
He won the third-tier Conference League with Roma in 2022, but his time at the Italian club from 2021 to 2024 was marked by squabbles that resurfaced in his brief and chaotic spell with Fenerbahce in Turkey.
His stint with Fenerbahce then came to an end last month after the Turkish club were eliminated by Benfica in a qualifying play-off of the Champions League.
Mourinho confirmed that Benfica had contacted him about their coaching vacancy.
"When I was confronted with the possibility of coaching Benfica, I didn't think twice, in the sense that I was interested," he said.
Benfica fired coach Bruno Lage on Wednesday, a day after the team's 3-2 home loss to Qarabag in the Champions League. They had squandered a two-goal lead in front of their fans, prompting club president Rui Costa to fire Lage.
Costa said it was a matter of great pride to have Mourinho back with the club.
"We wanted a coach who was a winner and we likely would not find one with a greater resume than Mourinho," Costa said.
Benfica's next match is on Saturday in the Portuguese league at AVS with their next Champions League game being at Chelsea, where Mourinho enjoyed his most sustained success as manager, on September 30.
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