Kevin Davies lashed the opener against Inter Milan's midweek conquerors from 18 yards and Gretar Steinsson screwed in an angled drive to make it 2-0.
Davies then added a penalty after Lee Chung-Yung had been felled in the box.
Alan Hutton's curler and a fine volley from Roman Pavlyuchenko threatened a late comeback, but Martin Petrov slid in a late fourth to seal Bolton's win.
It was no less than the hosts' effervescent and committed performance warranted, while questions must be asked of Tottenham's ability to juggle their European and domestic commitments following another post-Champions League defeat.
After the exhilarating high of Wednesday's win over Inter Milan, a trip to the Reebok Stadium was always going to have an element of 'after the lord mayor's show' about it - and the north Londoners' cause was not helped by the absence of injured pair Rafael van der Vaart and Aaron Lennon.
But Spurs boss Harry Redknapp has made no secret of the fact the league remains his side's top priority this season and he cut a frustrated - and at times furious - figure on the touchline as Bolton outfought and outplayed the visitors for long periods.
As early as the first minute Matty Taylor, preferred to the fit-again Petrov, could have opened the scoring when he blazed a great chance over the bar from inside the area, while Johan Elmander screwed wide when well placed.
With Steinsson and Lee doubling up on Gareth Bale and Niko Kranjcar misfiring, Tottenham's threat in attack was far more muted, though Sandro should have done better when set up by Wilson Palacios on the edge of the area.
Still, when Bolton's opener did come, there was an air of controversy about it.
Fabrice Muamba robbed Sandro in the middle and Taylor slipped the ball through to Davies, who - a yard offside - collected and slammed low into the corner.
Tottenham reacted well with Peter Crouch inches away from sliding a Bale cross home from inside the six-yard area and William Gallas forcing a sprawling save from Trotters goalkeeper Jussi Jaaskelainen with a left-foot curler.
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But the home side were well worthy of their half-time lead, and they picked up where they left off at the start of the second period, relentlessly harrying the Spurs midfield and centre-halves Gallas and Younes Kaboul.
Tottenham did come close to levelling the scores when Bale's wicked free-kick crashed against the angle of post and bar, but moments later they were 2-0 down when Steinsson capped a fine display with a rifled shot into the corner from Elmander's cut-back.
As they did after going 1-0 behind, Spurs sparked into life, and Sandro should have done much better with his finish six yards out from Alan Hutton's cross.
Kranjcar, too, found himself in space in the box from substitute Pavlyuchenko's pass - but could only blaze wildly over the bar.
However, Bolton continued to look a threat whenever they pushed forward and after Taylor hit the post with a left-foot snap-shot, Fabrice Muamba burst into the box only to put his shot into the side netting.
The home fans did not have to wait long for a third, though, and after Benoit Assou-Ekotto bundled Lee over in the box, Davies expertly dispatched the penalty.
Tottenham have yet to manage a single win at the Reebok in the Premier League - and for a time it looked like the hosts would run riot, Elmander forcing keeper Heurelho Gomes into a smart save at the Swede's feet.
To their credit, Reknapp's side rallied late on.
First Hutton surged infield from the right before curling a lovely finish left-footed into the far corner, and then Pavlyuchenko crashed home a stunning volley from the angle after Bolton could only half-clear Bale's free-kick.
And with three minutes plus stoppage time still to play, it briefly looked like Tottenham could snatch a dramatic draw.
But substitute Petrov put paid to any chance of that when he strode on to Davies' flick and prodded under the advancing Gomes to send the crowd into raptures and secure the three points that moved Owen Coyle's side above Tottenham in the league.