Under Gilbert’s tutelage, Gauff, 20, won her first major of the year in New York last year.
However, Emma Navarro, another American, defeated her in the fourth round this year.
“Coco, you have an incredibly bright future at just 20 years old, and I wish you nothing but continued success ahead,” wrote Gilbert on X. Gilbert also coached Andy Murray, Andy Roddick, and Andre Agassi, three past Grand Slam winners.
“I’m excited for the next chapter in my coaching career.”
Gilbert was brought on by Gauff to work with Spanish coach Pere Riba following a disappointing first-round loss at Wimbledon earlier this year.
Following that, Gauff’s fortunes took a turn for the better as she won 18 of her next 19 games during her home hard-court trip, culminating in titles in Washington, Cincinnati, and New York.