Twice grand slam winner Murray lost the Madrid Open final to Novak Djokovic on Sunday.
“I’ve learned a lot from Amelie over the past two years,” Murray said in a statement.
“She’s been a calming influence in the team and we’ll 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.”
Mauresmo described working with Murray as being a fantastic experience.
“I’ve thoroughly enjoyed being part of the great team of people he has around him,” she said.
“Dedicating enough time along with the travel has been a challenge for me. I wish him and the team well and I hope he goes on to win any more titles.”