Murray lost in the final of the Madrid Open against No.1 Novak Djokovic on Sunday and dropped to third in the rankings. The partnership between Amelie and Andy saw the Scot regain the world number two slot in the rankings earlier.
Since he began working with her in June 2014, Murray has won seven titles - including his first two on clay court - but has failed to add to his two Grand Slams.
“Working with Andy over the last two years has been a fantastic experience for me”, said Mauresmo in a Facebook post on Monday.
“I’ve thoroughly enjoyed being part of the great team of people he has around him. Dedicating enough time along with the travel has been a challenge for me. I wish him and team well and I hope he goes on to win many more titles.”
Murray said: “I’ve learned a lot from Amelie over the last two years, both on and off the court. She’s been a calming influence in the team and we will all miss having her around. I’ll take some time to consider the next steps and how we progress from here, but I’d like to thank her for everything she has done, she’s been an invaluable member of the team.”