Jermain Defoe scored a first-half penalty against former club Tottenham before Peter Crouch added a second to leave Juande Ramos' hapless side rooted to the bottom of the Barclays Premier League.
After gaining just two points from the first six matches Ramos was subjected to chants of "You don't know what you are doing" from fans after he took 73 minutes to send on top-scorer Darren Bent for lone striker Roman Pavlyuchenko.
But for Pompey it was a welcome return to winning ways having conceded 10 goals in their previous two matches, although the victory was tarnished when Lassana Diarra was sent off after a second yellow card foul on fellow Frenchman Benoit Assou-Ekotto two minutes from time.
For the second Sunday running Spurs could point to a harshly-disallowed penalty claim when substitute Aaron Lennon, felt he had been pulled down in the area against Wigan last week, saw his cross-shot clearly handled by Diarra in the 53rd minute.
The visitors had worked their way back into the game after Defoe's opener but were finished off Armand Traore, on loan from Arsenal, hit a thunderous shot which goalkeeper Heurelho Gomes parried for Crouch to head home his first Fratton Park goal since his summer move from Liverpool.
Defoe was on a mission from the start to prove a point to the club which sold him to Pompey in January.
Having been pulled up by an offside flag after just two minutes when he swept home Crouch's through-pass, the England international went on a one-man crusade against Spurs.
His 34th-minute penalty, awarded for handball by stand-in Tottenham captain Jermaine Jenas, must have felt sweet but he chose not to celebrate in front of the Tottenham fans packed behind Fratton Park's Milton End goal.
Defoe, however, must have been bubbling inside - just as Spurs seemed so flat.
They posted £14million Russian Pavlyuchenko in a lone front-running role but struggled to make any impact in the first half against a defence containing a nervous-looking Sol Campbell - perpetually jeered by Tottenham fans who still can't forgive him for leaving the club for Arsenal eight years ago.
James finally had a shot to save in the 26th minute but it was a tame effort by Jamie O'Hara, who should have done much better from a central position 14 yards out.
As James carried the ball away, Jonathan Woodgate bumped into him from behind and was booked - although it looked like an accident, caused by the goalkeeper's swerve before kicking clear.
O'Hara was booked in the 33rd minute for a foul on Little, who swept the free-kick into the area where Jermaine Jenas was harshly adjudged by referee Mike Dean to have handled the ball.
But that did not worry Defoe, who stepped up to bury the spot-kick past Gomes and ambled away as though it was just what he had expected to achieve.
But joy must have been mixed with relief after he missed his spot-kick miss against Vitoria Guimaraes in the UEFA Cup on September 18.
The home fans' mood was lifted further with the unmarked Pavlyuchenko's reaction to a perfect O'Hara pass five minutes before the break. The Russian spun away from the flight of the ball, looking completely lost.
It summed up an opening 45 minutes when Gomes was regularly diving around area, stopping a Defoe flick, watching a Crouch header fly just over and then holding onto a well-struck strike by Richard Hughes, even though Crouch trod all over him looking for a rebound.
There was still no sting in the Tottenham attack even though they took a grip on the game in the second half. And the denied penalty shout seemed to take all the wind out of their sails again.
It was close to stoppage-time when James, who shipped 10 goals in Pompey's two previous outings, had his first serious save to make from the luckless Lennon's low drive, tipping it around a post.
Crouch's clincher was tarnished by Diarra's exit but even on a day when Pompey were apparently obliged to deny a report the club is for sale because of massive debts, their joy was unconfined again.Reuse content