The 29-year-old Germany international had one year left on his contract at the Signal Iduna Park.
Schurrle has spent the last two seasons on loan in the English Premier League with Fulham and in the Russian top flight with Spartak Moscow but he has not played since December last year because of fitness issues.
Schurrle joined Dortmund from Wolfsburg in the summer of 2016 for £27m and scored eight goals in 51 appearances for the club.
A Dortmund spokesman said: "Borussia Dortmund and Andre Schurrle - who was recently loaned to Spartak Moscow - have mutually agreed to cancel his contract that was valid until 2021.
"As a result the 2014 World Cup winner will no longer take part when Borussia's pre-season training begins on July 30."
'Looking back, it's been a time with a lot of ups and downs, and a valuable experience, both in the sporting sense but also privately,' Schurrle said in a statement on the club's official website.
'I'd like to thank the club's bosses and wish the club and its special fans all the best for the future.'
Schurrle previously spent a season-and-a-half at Chelsea and helped the Blues win the 2014/2015 Premier league. He earned a winners’ medal from Chelsea’s triumph despite leaving for Wolfsburg half-way through the season.
He was a member of Germany’s 2014 FIFA World Cup winning squad, supplying the assist for Mario Gotze’s winner against Argentina in the final.
