Germany's Vettel, who will be chasing his fourth pole in a row on Saturday and seventh of the season, was quickest in both sessions with fastest laps of 1:20.976 and 1:20.087 respectively.
Australian team mate Mark Webber was second quickest in the morning, with the Red Bulls nearly a second quicker than the rest, but Ferrari's Fernando Alonso split the pair on a warm afternoon at the Hungaroring.
"I think this morning didn't really give a clear picture of each team's pace, but this afternoon it was tighter," said Vettel. "The Ferraris seem very quick again here on both the long and short runs." Poland's Robert Kubica, preparing for the nearest thing to a home race with plenty of fans waving red and white flags, was third and seventh respectively for Renault.
Red Bull have started 10 of the 11 races so far on pole position but have failed to convert that advantage in qualifying into regular race day success.
Vettel has won twice and Webber three times but McLaren are leading both Formula One championships with Lewis Hamilton and Jenson Button.
World champion Button, who took his first grand prix win with Honda in Hungary in 2006, was fourth fastest in the morning while Hamilton was 18th.
Hamilton is 14 points clear of Button with eight races remaining with Vettel a further seven adrift.
The overall leader, twice a winner in three visits to Hungary, improved to sixth after lunch but was in no doubt about the task facing McLaren.
"We've got a lot of work to do and I guess this weekend's just about scoring as many points as we can and hoping that the guys ahead have troubles," said Hamilton. "I think being in the top five could be tricky this weekend." Team boss Martin Whitmarsh said McLaren had made a few changes to their Friday programme, carrying out some shorter runs in the morning, but was surprised by their rivals' pace.
"While we're encouraged by both drivers' feedback, and by the overall balance of the car, the pace of the front-runners was somewhat unexpected," he said.
Alonso was a controversial winner in Hockenheim last weekend, after Massa was instructed to let him pass for victory.
Ferrari were later fined $100,000 for using banned team orders.
"Obviously they (Red Bull) seem stronger than in Hockenheim.
We know that we need to do something good tonight if we are to fight for pole position tomorrow," said the Spaniard.
Massa was back on track at the Hungaroring for the first time since his big accident in qualifying for last year's race.
The Brazilian wasted no time in getting in the groove, completing the first timed lap of the session.
