Scoring an impressive 114 in the Bonus Points System (BPS), Kane also supplied an assist and four completed dribbles.
Son Heung-min’s (£7.2m) contribution was largely overshadowed, although with 47 in the BPS, his brace of goals did earn the South Korean two bonus points.
Left wing-back Ben Davies (£5.0m) claimed the final bonus point on offer.
He supplied three open-play crosses and four key passes, one of which set up Kane for his fourth goal.
Davies scored 32 in the BPS, having also contributed five recoveries and three successful tackles.
Kane dominated in the ICT Index scoring his season-high tally of 31.1.
His Threat score of 124 was made up of 10 shots on goal, four of which arrived from within the Leicester City penalty area.
Since his first start on returning from injury in Gameweek 33, Kane has fired a total of 34 shots on goal, with 19 finding the target – 14 and 10 more than any other FPL forward respectively.
Meanwhile, Davies achieved the highest Creativity score (63) in Thursday’s contest.
Taking set-pieces in the absence of Christian Eriksen (£8.9m), the Welshman put in eight crosses in total, five of which found a team-mate.
Kane’s four goals provided a late and major upheaval in the FPL ranks, with his 24 points the biggest score achieved by a player in a single match this season.
That took him to 31 points over his two Gameweek 37 fixtures.
Part of 896,000+ squads, Kane was captained by just 26.2% of those owners and 5.5% of total FPL managers.
Some 15,194 managers made Kane their Triple Captain, representing just 6.1% of the 245,534 who had that chip in play.
Significantly, the Spurs striker has also moved two goals ahead of Lukaku, and three ahead of Sanchez, in the race for the Golden Boot.
Elsewhere for Spurs, Dele Alli (£9.1m) was restricted to a single assist.
He has supplied a goal and two assists over his last six Gameweek starts – a spell in which Spurs have scored 15 goals.
Alli lost 42,000+ owners heading into Gameweek 37 and will likely suffer a decline again for the final day, with more than 26,000 moving him out ahead of Sunday’s 2pm BST deadline.
Manager Mauricio Pochettino took the decision to rest Eriksen to the bench, frustrating the Dane’s 837,000+ (18.5%) owners. It remains to be seen if he is recalled for the visit to KCOM Stadium.
Eriksen had returned points in six of his last seven Gameweeks prior to Thursday’s omission.