Reigning Premier League champion van Barneveld repeated his victory over the world number one in last year's final as a clinical performance saw van Gerwen suffer defeat for the first time this season, in his 11th game.
Van Gerwen recovered from early missed doubles to hit back from 2-0 down to level and was also all-square at three-all before van Barneveld pulled clear.
An 11-dart leg pushed van Barneveld 4-3 up before he punished three uncharacteristic misses at double top from van Gerwen by breaking throw on double ten, before finishes of 78 and another 11-darter sealed victory.
"I'm extremely happy and it was a really good game," said van Barneveld. "I was really focused on this game and my finishes helped me, as well as those two 11-darters.
"To beat Phil last week and now Michael, I'm really happy. They are the two best players in the world at the moment but I'm playing well and that's seven points from the last five weeks.
"Michael's had a tough week but he didn't play that badly. He missed some crucial darts in the second leg but I'm battling hard and I want to get into the top four and win this fantastic Premier League again."
Six-time Premier League champion Taylor, meanwhile, bounced back from two successive defeats as he picked up three points from a possible four at the GE Oil & Gas Arena, defeating Dave Chisnall 7-3 before sharing the spoils with Stephen Bunting.
Taylor took an early 3-1 lead in his clash with Chisnall, who cut the gap to 4-3 but was unable to level as the Stoke star pulled clear to take the points.
Taylor later returned to the stage against Bunting, but spurned ten match darts as he walked away with a draw.
Taylor again took a 3-1 advantage and also held a 5-2 cushion before Bunting hit back to level with a 132 checkout.
Taylor then finished 64 to move 6-5 up and secure a point, and he first in a 177 in the deciding leg to be first to a finish only to see ten match darts miss their intended target, allowing Bunting to snatch a draw.
"I'm really pleased to come up to Aberdeen and take three points," said Taylor. "In the first game I got stuck in because I knew Dave was going to play well and I knew what I was up against, but I'm fighting for survival.
"Barney caned me last week but I'm better than that and I had to go out and perform tonight. I'll be there or thereabouts but I think with it being so close it's given us all a kick up the backside and it's interesting."
Bunting had earlier suffered a 7-2 defeat to Adrian Lewis as the two-time World Champion continued his revival with a third successive victory.
Lewis streaked into a 4-0 lead by punishing some early missed doubles by Bunting, who won two legs from three to hit back before the Stoke ace picked up both points.
"I'm happy with that because it was a big game that I didn't want to lose," said Lewis. "Stephen missed a few doubles early on but I was there on his tail, I kept calm and got the job done.
"I've done a lot of work on my game recently and it's showing in my results. It puts me in the mix for the top four and I think it will be between me and him for taking a point."
The night also saw World Champion Gary Anderson hit back from 6-2 down to claim a draw with James Wade, delighting the sell-out crowd who gave a memorable welcome to the Scottish star.
Wade had silenced Anderson's home support by taking a 2-0 lead, with the world number three hitting back to level only to be punished for missed doubles as the left-hander took the next four legs - and finished a brilliant 170 checkout - to claim a point.
Anderson, though, hit back strongly to take the next two and punished one missed match dart at tops from Wade by forcing a deciding leg in which he landed a fifth maximum of the game and tops to secure a draw.
"I was playing okay but a couple of missed doubles cost me a few legs and the next thing I knew I was 6-2 down and looking at a defeat, so I'll take the point.
"I had to stick in after his 170 finish and I got my scoring going again. It was nice to give the fans something to cheer because the fans in Aberdeen create a great atmosphere."
2009 Premier League champion Wade admitted: "It should have been two points but it wasn't. Gary missed a lot of shots but I played okay - I didn't play great - and I'll move on from here."
The Betway Premier League continues at the Motorpoint Arena in Cardiff next Thursday, with Anderson and van Gerwen set to compete twice on the night in Wales.
Betway Premier League
Night 11, Thursday April 16
GE Oil & Gas Arena, Aberdeen
Dave Chisnall 3-7 Phil Taylor
Stephen Bunting 2-7 Adrian Lewis
James Wade 6-6 Gary Anderson
Raymond van Barneveld 7-3 Michael van Gerwen
Stephen Bunting 6-6 Phil Taylor
Dave Chisnall v Phil Taylor
1-0 - Chisnall wins the opening leg in style with a 128 checkout, finishing two treble 18s and double ten.
1-1 - Chisnall misses double eight to break throw, allowing Taylor to return from a miss at tops to hit the bed and level.
1-2 - Taylor posts double 16 to break throw and move ahead.
1-3 - The pair trade 180s to leave finishes, with Taylor taking out 81 on the bull to take a two-leg lead.
2-3 - Taylor scores 100, 180 and 177 to leave 44 after nine darts - only to see Chisnall take out 140 for a 12-darter to hit back.
2-4 - Taylor opens with a maximum before finishing double 16 to regain his cushion.
3-4 - Chisnall replies in similar manner, kicking off the leg with his second 180 of the game before double nine sees him respond.
3-5 - Chisnall fires in a 180 to leave 38, but Taylor is already waiting on 24 and finishes double 12 for a 14-darter.
3-6 - Taylor seals at least a point with another 14-dart finish, opening with five perfect darts by scoring 180 and 140 before punishing one miss from Chisnall, at tops, by breaking throw for a second time.
3-7 - Taylor lands a fifth maximum, and when Chisnall misses one more dart at tops the Stoke ace steps in to seal victory on double eight.
Stephen Bunting v Adrian Lewis
0-1 - Lewis finishes 81 on the bull to break throw in the opening leg.
0-2 - Bunting sets up 16 with a 168 score, but misses three darts to level as Lewis steps in to finish 68 on double four to move two legs up.
0-3 - Bunting pays for three further missed doubles, allowing Lewis in on double 18 for another break of throw.
0-4 - The pair open with 180s, but Lewis wins a fourth successive leg by landing tops.
1-4 - Bunting misses the bull for a 161 finish, but is able to return and land double eight to get off the mark.
1-5 - Lewis opens with a 177 and punishes two misses from Bunting, who is unable to land darts at double 16 and eight, by finishing double four.
2-5 - Double 16 sees Bunting hit back.
2-6 - Lewis opens with five perfect darts of 180 and 140 before finishing double 12 to secure a minimum of a point.
2-7 - Lewis initially misses double 11 to finish 124, but returns to land double four to complete the win.
James Wade v Gary Anderson
1-0 - Anderson opens the game with a 180, but Wade adds a maximum of his own before landing tops for an 11-darter to take the lead.
2-0 - Anderson misses two darts at double 19 to level, and Wade returns on double ten to claim a break of throw.
2-1 - Anderson hits back with a break of throw of his own, landing double ten to get off the mark.
2-2 - Both players open the leg with maximums before Anderson lands double top to level the contest.
3-2 - Wade finishes 46 to regain the lead.
4-2 - Anderson misses two darts at tops to finish 100, and Wade steps in to break throw by hitting the same bed.
5-2 - Anderson lands his third 180 of the night, but again has trouble with double top - missing two further darts at the bed - to allow Wade to cash in once again on tops.
6-2 - Wade takes out a stunning 170 checkout to ensure that he will take at least a point.
6-3 - Anderson fires in a fourth 180 and breaks throw to keep the game alive on double four.
6-4 - Wade lands a 180, but Anderson takes out 81 for an 11-darter to close the gap to two legs.
6-5 - Anderson misses the bull to take out 121, but Wade is unable to land a match dart at tops to complete a 120 combination, allowing the Scot back in on double 12 to claim a point.
6-6 - Anderson posts his fifth 180 of the game to leave 78, before finishing tops to claim a point from a four-leg deficit.
Raymond van Barneveld v Michael van Gerwen
1-0 - Reigning champion van Barneveld takes the opening leg.
2-0 - van Barneveld breaks to double his lead.
2-1 - van Gerwen finishes 87 on double eight to hit back with a break of throw.
2-2 - van Gerwen levels by finishing 12.
3-2 - van Barneveld takes out 92 on double 18 to move back ahead.
3-3 - van Gerwen finishes 121 on double 18 to level.
4-3 - van Barneveld produces a superb 11-darter, hitting two 180s before finishing 41 on double 16.
5-3 - Three misses at double top from van Gerwen are punished as van Barneveld takes out double ten for a 14-darter to break.
6-3 - van Barneveld secures a minimum of a point by finishing 78 on tops
7-3 - van Barneveld scores 180, 140 and 123 before finishing an 11-darter to end van Gerwen's unbeaten run this season.
Stephen Bunting v Phil Taylor
0-1 - Taylor opens with three 140 scores, and has enough cushion to initially miss six darts at double 16 before hitting the bed to break throw immediately.
0-2 - Taylor lands a 180 and finishes double 16 to move two legs up.
1-2 - Bunting opens with a maximum before finishing 64 on double eight to get off the mark.
1-3 - Tops sees Taylor regain a two-leg lead.
2-3 - Bunting finishes 63 on double 16 to hit back.
2-4 - Taylor lands a 174 as he regains his cushion.
2-5 - Taylor fires in a 180 and double six to move three legs clear with another break of throw.
3-5 - Bunting posts a 180 and takes out 70 to punish Taylor for a miss at double 16 to complete a 112 combination.
4-5 - Taylor lands a maximum, but Bunting finishes double 16 to continue his revival.
5-5 - Taylor fires in his fourth maximum, only to see Bunting take out 132 on the bull to level the game with his third successive leg.
5-6 - Bunting misses double 16 to move ahead in the game, and Taylor takes out 64 on tops to break throw and secure at least a point.
6-6 - Taylor produces a superb 177 score to leave 88, before a dramatic deciding leg sees him miss ten match darts to allow Bunting back from six misses of his own to claim a draw on double one.