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Mourinho won the Premier League three times when Chelsea manager and, while Neville does not believe Spurs will end up champions, he acknowledges the former United boss has the attacking power at his disposal to deliver a first league title for the north London club since 1961.
"I said a couple weeks ago on Monday Night Football that Spurs couldn't win the league, and I still don't think they can,” the former United defender told The Gary Neville Podcast.
"But I do agree with Jamie Carragher that it would be the most outstanding story to see Jose Mourinho win the Premier League with Tottenham.
"It would be something that would alarm Chelsea fans, Manchester United fans and Arsenal fans. It would be one of the great stories, because Tottenham don't win leagues!
"He's got the forward players to do it. You think of the strike force and the goal - it's incredible.”
Neville also praised Harry Kane, whose winner against West Brom was his 150th goal in the Premier League, which came a few days after hitting the 200 mark for Spurs.
He added: "The only thing that can stop Harry Kane doing everything in the game, breaking every record, is injury.
"Alan Shearer is definitely the best striker in PL history in terms of his goal record. He's the best striker I've played with for England, in terms of a number nine, and Rooney I'd put up there with him.
“And Harry Kane has so much similarity in his game, in terms of the mentality, just ice cold, doesn't seem to flinch if he misses a chance, flinch if a goalkeeper saves one, he'll come back and do the right thing. Scoring a goal is a process for them, where he knows where the target is.