Already a force at just 18, Littler now sits on 35 points and is within striking distance of smashing the record for the highest-ever points total in Premier League history.
Van Gerwen, determined to halt Littler's march, burst out of the blocks in the final with a commanding 3-1 lead, including a sharp 76 checkout.
But Littler, unshaken, responded with a stunning 120 checkout that brought him back into the contest before he coolly levelled things up at 3-3.
With momentum shifting, Littler surged ahead with an 81 checkout, but Van Gerwen responded with a tidy 14-darter to square it again.
However, the final stages belonged to Littler. He pinned his trademark double 10 to edge closer to glory and, when MVG faltered on his throw, 'The Nuke' sealed the victory on tops - writing another thrilling chapter in his already glistening career.
"I'm very happy," Littler told Sky Sports after the record-breaking victory.
"The fifth nightly win was going to come at some point, but it's been a few weeks since I actually won on a Thursday.
"But winning tonight, I'm nine points clear, so I'm very happy and very confident I'll stay at number one.
"There are still a few weeks left to play. It's getting a bit nitty, gritty at four and five between Nathan and Michael, so I've done Nathan a favour by winning this one.
"I'm still looking at three, four and five. It's going to be a good few weeks watching them guys fight for the top four while I'm cruising at the top.
"I've enjoyed it right the way through, but I'll certainly relax."
Earlier in the night, Littler was forced to dig deep against Stephen Bunting.
After falling 2-0 behind, he clawed his way back, producing a sublime 11-darter to force a decider.
Calm and collected, Littler held his nerve in the final leg to edge Bunting 6-5 and kickstart another magical run.
The semi-final against Nathan Aspinall proved just as dramatic.
Littler hit seven 180s and averaged 96.56 but had to survive a match dart from 'The Asp' before closing it out in a nail-biting decider.
Aspinall pushed Littler to the brink, but the young star's sensational 174 setup shot and clutch double 10 finish sent him through to his seventh Premier League final this season.
Elsewhere, Gerwyn Price delivered a statement win against Luke Humphries, overturning a 5-3 deficit with a clinical 102 checkout. Price's reward was a semi-final clash with Van Gerwen, who had earlier kept his play-off hopes alive by dispatching Rob Cross with a superb 130 checkout.
Van Gerwen scraped past Price in a scrappy semi-final, surviving seven missed match darts from the Welshman to reach the final.
The Premier League continues with Night 14 at the First Direct Arena in Leeds next Thursday.
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