Damion Stewart headed home after 58 minutes to put the Championship side into the fourth round as a reshuffled Villa side struggled to find any fluency.
Barry was one of only five survivors from Villa's Premier League victory over West Brom and was asked to lead the side for the first time since his dream move to Liverpool fell through.
But despite a lively display from Ashley Young, Villa could not find the goal they needed to force extra-time.
Carlos Cuellar was handed a first home start alongside Zat Knight in a reshuffled Villa defence, while Isaiah Osbourne and goalkeeper Brad Guzan, on debut, were given chances to impress.
The applause when Barry's name was announced to the fans was warm, if a little less than delirious, but the decision suggests that, if any further proof were needed, player and manager are fully reconciled.
Villa had a gilt-edged chance to open the scoring in the 10th minute after fine work down the left from Barry and Nicky Shorey provided Stiliyan Petrov with possession just outside the box.
The Bulgaria international opted not to shoot, instead rolling the ball delicately into Marlon Harewood's path only for the striker to curl his effort over the crossbar from six-yards out.
Emmanuel Ledesma, scorer of a hat-trick in the previous round, showed some neat footwork inside the Villa box to give the hosts a scare but he ran the ball a fraction too far and lost sight of goal.
Young then showed the skill and fleet of foot that mark him out as an England star in the making when he set in motion another Villa attack with a first-time flick with the outside of the boot.
That set Barry scampering down the flank but when he found Harewood in the middle, he could not steer his shot through a clutch of hooped shirts.
Young, predictably, was involved in Villa's next good chance, springing the offside trap before trapping the ball on the touchline and drilling it into the box.
His pass took a deflection before finding Harewood, who snatched at a tough chance and powered it into the stand.
Cuellar, who looked short on composure in his first home start, was booked 10 minutes before the break for dissent.
Young, the liveliest player on the pitch by a handsome margin, looked as though he would send Villa into the break ahead but his sweetly-hit effort curled just wide of the far post.
Osbourne, like Cuellar, appeared to be fluffing his lines on what could be seen as an audition for the first XI, betraying a poor first touch seconds after the restart and immediately ceding possession.
Villa quickly cranked up the pressure, Young earning a corner with a low near-post cross from the right which Harewood might have done better from.
Then, with 58 minutes on the clock, Rangers took an unlikely lead.
The away side won a disputed corner and although that was cleared, Daniel Parejo - on loan from Real Madrid - floated the ball back into the penalty area where Stewart rose to nod a bullet header beyond Guzan.
Panic appeared to be spreading in the home ranks, with a series of mis-hit passes and poor touches serving to spur on their opponents.
With a little over 23 minutes remaining, O'Neill sent on Gabriel Agbonlahor and Wayne Routledge.
O'Neill had probably been hoping to give Agbonlahor, who has endured a heavy workload so far this season, a night off but summoning him from the bench was an obvious show of intent.
After 75 minutes, the chance of an equaliser came and went as Barry spurned the chance to cap his return as skipper with a goal.
Carew flicked on a high ball leaving the onrushing Barry clear on goal. The England midfielder opted to chip the advancing Cerny but failed to hit the target.
It did not get any better for Villa, who by now were tossing away possession liberally.
Routledge screwed a presentable chance wide with three minutes to play, ending Villa's hopes of a sixth League Cup with a whimper.
| Today's other Carling Cup matches. | |||
|---|---|---|---|
| Blackburn | 1 - 0 | Everton | Report |
| Olsson 10 | Att: 14366 | ||
| Ipswich | 1 - 4 | Wigan | Report |
| Walters 61 | Cattermole 52 Kapo 64 Scharner 70 Camara 90 | Att: 13803 | |
| Newcastle | 1 - 2 | Tottenham | Report |
| Owen 90 | Pavlyuchenko 62 O'Hara 66 | Att: 20577 | |
| Portsmouth | 0 - 4 | Chelsea | Report |
| Lampard 36(pen),49 Malouda 45 Kalou 64 | Att: 15339 | ||

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