The Lilywhites found themselves two goals to the good midway through the high-intensity match following an impressive first-half showing at White Hart Lane, with the visitors unable to find a way back into the contest in the remainder as they slipped to a 2-0 reverse.
Pep Guardiola therefore misses out on the chance to become the first manager in Premier League history to win each of his first seven games in charge, falling short of hitting that target and making it two games without a win for his side now in all competitions.
Spurs climb back up to second place, meanwhile, with five wins in succession in the top flight - and a third in a row against City - enough to keep them right in the mix at the top heading into the two-week international break.
Mauricio Pochettino's side looked to get right in their opponents' faces from the off, fashioning a chance through Son Heung-min with 20 seconds on the clock which the in-form forward could only flash wide.
The hosts did not have to wait too long to make a breakthrough, however, as Victor Wanyama's impressive work in midfield to win back possession created an opening for the returning Danny Rose to swing a cross into the box, which Aleksandar Kolarov sliced into his own net.
Son, with five goals in five games this season heading into this one, could have added a quick-fire second but he was unable to beat Claudio Bravo at the near post just moments after seeing his side make the breakthrough.
Spurs were continuing to dominate things, not allowing the Citizens a chance to settle and coming close to a second when Christian Eriksen sent a free kick just inches wide of the target with a quarter of the game gone.
City showed the occasional sign that they were slowly starting to grow into the contest, though their only shot of any sort in the first half was simple enough for Hugo Lloris to keep out at the end of a tame Sergio Aguero set-piece attempt.
Dele Alli added a deserved second for the Lilywhites eight minutes before half time, with Son picking out his teammate with a fine through-ball for the Englishman to tuck past Bravo to put City on the brink of their first league defeat under Guardiola.
Despite his side needing a few goals to keep that perfect domestic start intact, Guardiola decided to wait until 15 minutes into the second half before bringing on Ilkay Gundogan in place of Fernando in his first alteration.
Spurs perhaps should have been three to the good by that point as Son once more found himself in acres of space but could only curl his attempt wide, while Wanyama's shot from the edge of the box needed the slightest of touches from Bravo to help it wide.
City did hit the post shortly before the hour when Aguero's shot deflected off Lloris and onto the woodwork, but Spurs were given a glorious chance to settle things for good when Fernandinho bundled over Alli inside the box 25 minutes from time.
In the absence of Harry Kane it was left to Erik Lamela to take on spot-kick duties, though his penalty lacked both pace and precision which made life far too easy for Bravo who guessed the right way to push the ball aside.
Guardiola next turned to Kelechi Iheanacho as his charges desperately tried to build on their unexpected lifeline, and the youngster so nearly pulled one back when only denied by Lloris after being slipped through by David Silva.
City continued to push forward in the remaining 15 minutes, again testing Lloris through a deflected Aguero shot, but the division's most potent attack could not find a way past the division's strongest defensive unit.