The singer signed to Universal Music Group's Mercury Records in 2004 as part of Sugarland, when the band was a trio.
She also enjoyed solo success with the company.
In announcing her decision to move on in a statement to Billboard.com, Nettles says, "I want to thank Universal Nashville for 11 wonderful years. This change is the first step on a path I've been wanting to take. I am so excited about the next part of my journey and I invite my fans to stay tuned."
As a member of Sugarland, Nettles scored 11 top 10 hits and four platinum albums.