The 47-year-old had a contract at Signal Iduna Park that ran until 2018, but has been permitted to terminate his deal early.
Klopp stated that the decision was taken because he no longer felt he was the best coach for Dortmund.
"We've both invested a lot and got a lot back. No-one needs to be thankful," he said.
"I've said over the last few years that when I'm no longer in the best place to coach, I will say so.
"I chose this time to announce it because in the last years some player decisions were made late and you couldn't react.
"I definitely believe this to be completely the right decision. This club deserves a manager who is 100 per cent right for the club, and that's why I made the decision."
"This has nothing to do with me being tired," he added. "I read that this morning. I have not planned a sabbatical.
"My last wish is to finish the season in the highest possible position and that we can have an open-top parade with the cup."
Klopp, who joined from Mainz in 2008, is a popular figure at Dortmund having led the team to back-to-back league titles as well as completing a Bundesliga and DFB-Pokal double in 2012.
Dortmund also made the final of the UEFA Champions League under Klopp's stewardship in the 2012-13 season, but they were beaten by rivals Bayern Munich.
