The reigning world champion added the Night Eight crown to his earlier triumphs in Cardiff and Dublin, producing a series of high-class performances at the Uber Arena to overtake Jonny Clayton at the summit of the standings after the Welshman fell early to Josh Rock, handing the Northern Irishman his first win of the competition.
Littler opened the night with a 6-3 win over Stephen Bunting, coming through a high-quality quarter-final despite Bunting averaging 107.47. Littler himself averaged more than 105 in a strong display to reach the last four.
He then raised his level again in the semi-finals, beating Gerwyn Price after overturning a 4-3 deficit, averaging a mighty 108.58 to secure his place in the final.
Littler beats MVG again
That set up a decider against Van Gerwen, who had already recorded wins over Luke Humphries and Josh Rock to reach his third nightly final of the season.
Littler made the sharper start, moving 3-0 ahead and taking out 126 on the bull to put Van Gerwen under immediate pressure.
Van Gerwen responded well, reeling off three straight legs to level at 3-3, but Littler regained control at a crucial stage. A 170 checkout moved him 5-3 in front, and although Van Gerwen broke back to keep the match alive, Littler finished the contest in emphatic fashion with another 170 checkout to complete a 6-4 victory.
World number one Littler averaged 106.36 in the final and landed three ton-plus finishes in a performance he described as his best across a full night in this year's competition.
"Germany wasn't too bad tonight," Littler told Sky Sports afterwards.
"I played very well, and they were on my side at times. I reeled the 170s back in!
"I think this is definitely the best I have played in a night. I said coming in that if I won my first game, I would change my darts in the second. That will get a few people talking. Target did a few adjustments as they weren't quite right, but they worked tonight."
Van Gerwen's route to the final had been built on back-to-back 6-3 wins over Humphries and Rock. His finishing proved decisive in both matches, although an average of 103.87 in the final was not enough to stop Littler's charge to the title.
Rock records overdue win
Earlier in the evening, Rock recorded his first win in the Premier League by beating Clayton 6-3. The result ended a run of seven straight defeats for the Northern Irishman and denied Clayton the chance to remain top of the table.
In the other quarter-final, Price made an impressive return by defeating Gian van Veen 6-1 with a 101 average. It was his first appearance since undergoing surgery for kidney stones last week.
The result in Berlin leaves Littler two points clear of Clayton at the top of the table. Price sits third, with Van Gerwen in fourth, while Humphries is two points further back in fifth. Van Veen, Bunting and Rock remain in contention behind them.
The Premier League continues with Night Nine in Manchester on Thursday, April 2nd, where Littler will face Van Veen in a repeat of January's World Championship final.