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Mourinho was sacked by Tottenham last week after their form nosedived from mid-December, but he helped to bring out the best in Kane, who is on course to be the first player to finish as top scorer and with the most assists in the Premier League.
Mourinho, who promised to take Kane "universal" during a meeting in the manager's office shortly after his appointment in November 2019, allowed the England captain a free role and he has flourished when dropping deep.
"He is a fantastic manager," Kane said after last night's London Football Awards.
"He has managed the biggest players at the biggest clubs in the world. He came in with a real understanding of what he wanted. We had good conversations early on and that continued. I have always liked to drop deep, but the biggest change was to ensure people were running in behind if I was dropping deep.
"We just had a good relationship. I feel like my game has been evolving over the last three or four years anyway and it was just a good match-up. It was a shame that we could not go on and do better things or win any trophies, but I will take the experience I had with him for the rest of my career."
Mourinho was dismissed with Spurs seventh in the table and out of the FA Cup and Europa League, while they lost Sunday’s Carabao Cup Final to Manchester City.
Kane is still hoping Spurs can make it a more positive season by sneaking into the top four with the remaining five matches.
“If we win the last five games now and get good results from other teams and we somehow get into the Champions League then, obviously, it will be a bit of a brighter note,” he said.
“But all in all, we know we have got to definitely improve going into next year if we want any chance of trying to compete at the highest level.”