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The Tottenham striker also finished ahead of club-mate Heung-min Son and West Ham's Tomas Soucek to claim the honour after a remarkable season in which he remains in contention to finish as both top-scorer and with the most assists in the Premier League, despite Spurs' patchy form.
With five matches remaining, the England captain is leading the race for the Golden Boot with 21 goals and has the most assists in the top-flight with 13.
If he maintains both leads, he would be the first player to be complete the double in the Premier League era.
His remarkable output has been the highlight of an otherwise forgettable season for Spurs, who sacked manager Jose Mourinho last week before losing the Carabao Cup Final to Manchester City.
Kane's award was one of 10 announced on Tuesday night at a virtual ceremony hosted by Harry Pinero and Alex Scott, with Crystal Palace manager Roy Hodgson having already been recognised with the award for an Outstanding Contribution to London Football.
This year’s Awards are again in support of the charity Willow, which was founded by former Arsenal goalkeeper Bob Wilson.
Nominees were selected by an expert judging panel from the worlds of football and media, from former players to major footballing bodies and sports media, including The Evening Standard, Sky Sports, BBC, The Daily Telegraph and talkSPORT.