With the second phase of the tournament kicking off following last week's elimination of Peter Wright and Kim Huybrechts on Judgement Night, Chisnall and James Wade doubled up to compete twice in Sheffield.
Whilst Wade was defeated twice, Chisnall produced two outstanding displays as he overcame the left-hander 7-1 with a 114.17 average - his highest ever in a televised game - after earlier seeing off World Champion Gary Anderson 7-3.
That double earned Chisnall four league points to strengthen his position in second place in the league table - and crucially give him an eight-point cushion over his rivals battling for a Play-Off place.
Chisnall had landed key finishes of 150 and 124 as he turned a 2-1 deficit into a 5-2 advantage on his way to victory against Anderson, hitting six 180s and a 106.91 average.
He was in even more dominant form on his return to the stage against Wade, limiting the 2009 champion to only two darts at a double in a performance which saw his average second only to Phil Taylor in Premier League history.
Chisnall took the first five legs without reply and had missed double 12 for a 138 finish before Wade took leg six by finishing 62 - but the left-hander's fightback was short-lived as the St Helens ace posted a fifth 180 of the game in a 12-darter and double ten for a 14-darter to complete the win.
"It's nice to get two wins because it was always going to be hard," said Chisnall. "I felt comfortable throughout the night and I got a great start by defeating Gary.
"It was always going to be a confidence boost beating the World Champion and I just wanted to take the same game up on stage against James, which I did.
"I've done my job by winning two out of two, and I played well - importantly I finished well tonight. I felt good up on stage but I've put a lot of practice in and it's all working out.
"This time last year I was on seven points, so it's a big improvement to be up to 17 already!"
Chisnall now sits just one point behind the unbeaten league leader van Gerwen, who edged out Stephen Bunting 7-5 in their Sheffield encounter.
Bunting hit back from 3-1 down to lead 4-3 and 5-4, but he paid for missing a dart at the bull to claim a point in leg ten when van Gerwen levelled on double nine, hit two 180s to break throw with a 12-darter and then took out 70 for the win.
"I wasn't at my best tonight but I got the win and another two points so I'm happy with that," said van Gerwen. "I missed a lot of doubles but I produced the darts when I needed to.
"I let Stephen back into the game and he scored well, but at five-all I wanted to have one big leg and I started with 180 and 180, and the 12-darter was amazing for me and very important."
Wade's defeat to Chisnall compounded a disappointing night for the world number six, who also went down 7-4 to Adrian Lewis as the Stoke ace joined the left-hander and Taylor on nine league points in joint fourth place.
Lewis' win followed up his defeat of Wright to ensure that he avoided elimination a week ago, and has kick-started his own bid to claim a semi-final spot.
"I was happy with that win," said Lewis. "James wasn't at his best tonight but I did the job and it's a good win for me.
"I scored pretty consistently and kept the pressure on James, and when I needed a finish it went - some of my two-dart finishes were very good. I'm in contention for the top four now and I'm on the tails of the top four now."
Reigning champion van Barneveld sits just one point behind the trio on nine points after he overcame great rival Taylor 7-2 as the Stoke great suffered a fourth defeat in five matches.
Taylor had hit back from 2-0 down to trail just 3-2, but missed five darts to level the match in a key sixth leg and also missed tops in the seven as van Barneveld pulled clear to complete his first 'Premier League double' over the 16-time World Champion.
"To beat the best player in the world 7-2 is a dream and I'm extremely happy," said van Barneveld.
"Phil didn't play as well as he can and he missed a lot of doubles, which leg me in, but I was surprised by his game because we all know what he can play like. I had to keep trying to hit my treble 20s and take my chances when he gave me them.
"I was really focused because in all these years in the Premier League I'd only got two draws against Phil in the league stage but this year I've won twice, and in the last four weeks I've been playing okay.
"I'm fighting to get into the top four, and after tonight I believe it can be done."
The Betway Premier League continues at the GE Oil & Gas Arena in Aberdeen, with Taylor and Bunting playing twice on the night and World Champion Anderson up against Wade on home soil.
Betway Premier League
Night Ten, Thursday April 9
Motorpoint Arena, Sheffield
Adrian Lewis 7-4 James Wade
Gary Anderson 3-7 Dave Chisnall
Phil Taylor 2-7 Raymond van Barneveld
Stephen Bunting 5-7 Michael van Gerwen
Dave Chisnall 7-1 James Wade
Adrian Lewis v James Wade
1-0 - Wade lands a 162 score but misses four darts at doubles to break throw, allowing Lewis back to land double nine to claim the opening leg at his seventh attempt.
2-0 - Lewis fires in a 180 before finishing tops to break.
3-0 - Lewis wins a third successive leg to continue his fine start.
3-1 - Wade replies on double ten.
3-2 - The 2009 champion breaks throw with a 106 finish to continue his revival.
4-2 - Lewis breaks back, opening with a 180 before landing tops.
4-3 - Wade replies with a 14-darter, taking out 86 to reduce the gap to one leg once more.
4-4 - Lewis lands a maximum, but Wade finishes double four to level the game.
5-4 - Lewis fires in his fourth 180 of the game before hitting double top to edge back ahead.
6-4 - Wade misses the bull to finish 161, and Lewis takes out 67 in two darts to break and secure at least a draw.
7-4 - Lewis takes out 110 on tops to claim the victory.
Gary Anderson v Dave Chisnall
1-0 - Anderson finishes 60 on tops to take the opening leg.
1-1 - The pair trade 180s before Chisnall finishes double four to level.
2-1 - Chisnall misses tops to break throw, and Anderson returns on double five to move back ahead.
2-2 - Chisnall finishes a superb 150 checkout to hit back once more.
2-3 - Chisnall fires in a 180 before finishing 48 on double 16 to break and move in front.
2-4 - Chisnall lands another maximum before posting double four to win a third successive leg.
2-5 - Chisnall takes out 124 on double 11 to move three legs clear.
3-5 - Anderson opens with a 180, with Chisnall then landing two maximums only to miss a pair of darts at double 16, allowing the World Champion in on tops for an 11-darter.
3-6 - The pair again trade 180s, but Anderson is punished for two misses at tops as Chisnall seals at least a point with double 16.
3-7 - Chisnall completes victory with a supeb 14-darter, ending the game with a 106.91 average as he completes a seasonal double over Anderson.
Phil Taylor v Raymond van Barneveld
0-1 - van Barneveld lands a 180 and breaks by finishing 48 on double 16.
0-2 - The reigning Premier League champion doubles his lead by taking out 40 on double ten.
1-2 - Taylor replies by finishing 68 on double seven.
1-3 - van Barneveld finishes 92 on double 16 to move two legs clear again.
2-3 - Taylor finishes double 16 with his third dart as he replies.
2-4 - The pair both miss doubles across two visits, with five misses from Taylor punished by van Barneveld on double eight.
2-5 - van Barneveld lands a 180, and when Taylor misses tops to finish 114, the Dutchman steps in to hit the same bed.
2-6 - The reigning champion seals at least a point, landing a 180 and double eight.
2-7 - Taylor misses the bull to finish 170, and van Barneveld takes out double ten to complete the win - and take a league double over his great rival.
Stephen Bunting v Michael van Gerwen
1-0 - Bunting finishes 34 as he wins the opening leg.
1-1 - van Gerwen takes out 40 to level.
1-2 - The league leader lands his first 180 before punishing three missed doubles from Bunting to finish tops to break and move ahead.
1-3 - van Gerwen opens with 140 and 180 before landing double eight to move two legs clear.
2-3 - van Gerwen misses double 13 to finish 146, allowing Bunting to reply on double five.
3-3 - The Dutchman posts a 180 but misses double 18, as Bunting steps in to level by finishing 64.
4-3 - Bunting regains the lead, hitting a third 180 before finishing 69 on double 16.
4-4 - Double 17 sees van Gerwen level.
5-4 - Bunting opens with a 180 before finishing 72 on double 16 to move back ahead.
5-5 - Bunting fires in his fifth 180 of the game, but misses the bull as van Gerwen takes out 61 on double nine.
5-6 - van Gerwen sets up a possible nine-darter by opening with two 180s, and though he is unable to take out 141 he returns on double five for a 12-darter to remain unbeaten this season.
5-7 - van Gerwen, with the advantage of throw, takes out 70 in two darts on double eight to claim the win.
Dave Chisnall v James Wade
1-0 - Chisnall takes out 81 on the bull to claim the opening leg.
2-0 - Chisnall posts two 180s before finishing 83 to break throw and double his lead.
3-0 - Double ten sees Chisnall take a third successive leg.
4-0 - Chisnall posts a 168 score to leave 16 before double eight seals another break of throw - maintaining an average of almost 116.
5-0 - Another maximum helps Chisnall win a fifth leg, although Wade misses double 13 to finish 81 to allow his rival in on double eight.
5-1 - Chisnall opens with a 180, but misses double 12 to finish 138 to allow Wade in to take out 62 on tops to claim his first leg.
6-1 - Chisnall fires in his fifth 180 of the game before taking out 87 on double 18 to seal a point.
7-1 - Double ten seals a superb victory for Chisnall, who averages 114.17 - his highest ever on television and the second highest by any player this season.