The Frenchman made his debut for the team in 2012 and has impressed throughout his three years with Red Bull's sister team.
Seven points finishes last term continued his progression, but his performances were not enough to earn him another year, and there will be no reunion with Daniel Riccardo after he was snubbed by Red Bull in favour of 2014 colleague Daniil Kvyat.
Max Verstappen will become F1's youngest ever driver when he races for Toro Rosso in 2015, Carlos Sainz Jr - a member of Red Bull's young driver program - has been widely tipped to make the step up to join the Dutch teenager.
"Despite a good season and 22 points, I'll not drive anymore for Toro Rosso in 2015," Vergne posted on Twitter.
"Thanks for those years. Let's go for another big challenge."
It is unclear whether Vergne will move to another F1 team, though Sainz Jr currently has a chance to impress at the post-season testing in Abu Dhabi.
The Spaniard is currently testing Red Bull's 2014 car, and hopes his performances will lead to a spot with the secondary outfit within the organisation next year.
"I'm not hearing much, I'm just waiting for them to make a decision," he said.
"I'm sure they will make the correct one and obviously I would like that to be me. I don't know what can happen and I have to wait and see.
"This test was an important one for me to let them know the step forward I made from last year [when Sainz tested the 2013 Red Bull], for them to get to know me a bit better and hopefully they can choose me."