The 28-year-old singer took to Twitter on Saturday (11Jul20) to reveal the split, which makes him the fifth and final former One Direction star to depart their former "The X Factor U.K." mentor's company.
"Hope everyone is doing ok! Just wanted to let you know that Syco Music and I have agreed to part ways," Louis tweeted. "I'm really excited for the future and to be back in the studio writing the next album. Can't wait to finally see you all on tour!! Stay safe and see you soon, Louis x."
Louis and One Direction first signed with Syco after finishing in third place on the 2010 season of the TV talent contest and released five hit albums under the banner.
When the "Midnight Memories" hitmakers went on hiatus back in 2015, however, Louis was the only member to stick with Syco while Harry Styles, Liam Payne, Zayn Malik, and Niall Horan all signed with different labels.
Louis released his debut album, "Walls", through Syco earlier this year, peaking at number four in the U.K. and landing in the top 10 on the Billboard 200 in the U.S.