The striker scored either side of half-time to secure all three points for Spurs, sending them to within two points of Premier League leaders Leicester City, who will look to extend their lead back to five against Newcastle United on Monday, the Foxes' game in hand.
Despite that, it's a huge boost for Mauricio Pochettino's side after three games without a win, and they'll now hope to get their title chase back on track in the coming weeks.
Having rested a number of key players for the Europa League clash with Borussia Dortmund on Thursday, it was no surprise that a host of familiar faces came back into the starting XI, Dele Alli and Moussa Dembele amongst them.
Tottenham bang on the door...
It took just five minutes for Spurs to quieten an already disgruntled home crowd, hitting the bar. Erik Lamela slipped eventual goalscorer Kane in-behind the defence, but the striker wasted his first chance of the game, dinking the ball over Brad Guzan, only for it to strike the bar and go out.
Guzan was called into action for Kane's next opportunity, with the 'keeper's out-stretched leg denying the striker after he latched on to Danny Rose's cross.
Spurs had Villa on the back-foot for much of the first half, and edged even closer to an opening goal briefly after the half-hour mark, Alan Hutton clearing off the line. Kyle Walker angled a cross in for Lamela, who hit the post before the ball bounced off Guzan and looked to be rolling in, only for the Scottish international to sweep the ball away.
And Kane comes through the roof...
The hosts threatened little, their best chance of the first half coming towards the end of proceedings, as Hugo Lloris was equal to a Rudy Gestede header. They were soon behind, as Kane struck. Dele Alli was on hand to provide the assist, sending a quick free-kick into Kane's path, and the frontman showed excellent composure to beat Guzan at his far post.
That goal came in the third minute of added time, and Kane's second came in just the third minute of the second half, virtually sealing the win against a despondent Villa. Alli to Kane was the combination again, the midfielder finding his mate with a cross from the left wing - the striker only too happy to poke into the top corner for his 19th of the league season.
An unmarked Kyle Walker had a powerful drive saved by Guzan as Spurs attempted to make it three, before the tempo lulled slightly, only for Villa to have a bright spell right at the end of the game.
Villa's late spell won't be remembered
Jordan Ayew, disappointing again as he eases his way back from suspension, struck the post with an effort, the ball falling to Rudy Gestede - only for him to hit the bar from the rebound. Gestede then turned provider, flicking on to Joleon Lescott from a corner, but the defender couldn't get his effort on target.
Despite a late flurry from Villa, the three points were Tottenham's, and that's all that mattered.