The 32-year-old has opted not to extend his contract with the club next summer and instead will move into an advisory role helping to manage the careers of professional athletes.
A tough decision
"The decision to give up football wasn't one that I made lightly," said the former SV Werder Bremen trainee to bayer04.de. "I've been in football for 15 years and I've seen a lot of things and developed other interests. Now I think the time has come for me to call time on my playing career and continue to develop myself professionally as well as personally.
"My time at Leverkusen has really left an impression on me. Bayer are one of Germany's top clubs and always play in Europe. I became a Germany international and played in the Champions League here. I'm grateful to everyone at the club for everything they've done for me. In the summer I'll look back on ten eventful years at this club."
Völler: 'Door is always open'
"Simon gives our team structure with his experience and quality," said sporting director Rudi Völler. "He was one of our most important players in the early part of this season, and he could certainly play for another few years at the highest level. Even if he has many other plans next summer, the door will always be open for him at Bayer 04."
Rolfes has made a total of 269 appearances in the Bundesliga - all of them for Bayer 04 Leverkusen, whom he joined in 2005 - and scored 40 goals. He also represented Germany on 26 occasions, helping die Nationalmannschaft finish runners-up at UEFA Euro 2008.