Teddy Sheringham had previously held the record of 97 goals in England's top flight for the club, but Kane met and surpassed the tally with his double, tapping home early in the second half (47) before bobbling the record-breaking goal into the net 12 minutes later.
Pochettino said: "He is fantastic and he deserves all the credit and all the praise, so I want to congratulate him one more time".
"It is unbelievable the way that he is able to work and his willingness. He's always thinking and trying to improve, improve, improve and score goals".
Heung-min Son opened the scoring before Harry Kane bagged a brace in the second half to put Spurs 3-0 up.
It hardly mattered, however, as Kane extended Spurs' lead moments later with a close-range finish over Pickford from Eric Dier's precise pass into the box.
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He threatened to ruin his legacy among Barcelona fans though when he jumped ship for Ligue 1 giants PSG five months ago. However, former Barcelona star Ronaldo believes the move was a step down in terms of his footballing development.
"You've got to make sure you defend even better against [the likes of] Tottenham when they go 2-0 up and not relinquish that defensive responsibility, otherwise you get what what we just got. Hopefully I'll keep scoring".
In a unusual game that ebbed and flowed, Wayne Rooney had the first chance after a quiet opening, with the striker latching onto a long kick from Jordan Pickford and dragging a left-footed shot wide of the right post from inside the area on 16 minutes.
West Bromwich Albion claimed their first win under Alan Pardew with a 2-0 victory over Brighton thanks to goals from Jonny Evans and Craig Dawson.
"On my understanding he wasn't included in the 25 man squad at the start of the season, he hasn't been training with us for that period", Allardyce explained.
"Or what would the game have gone like if Harry's goal would have been disallowed - because I think it's offside looking on the laptop".
"I can't excuse our capitulation after we went 2-0 down".