Amélie Mauresmo has been by the British number one’s side since the summer of 2014, with former French professional credited with helping improve Murray’s performances after his return from a back injury.
But their parting of ways comes after Murray was beaten in the Madrid Open final on Sunday by Novak Djokovic, a defeat which saw him lose his world number two ranking to Roger Federer.
It throws into doubt Murray’s preparations for a busy summer schedule, during which he will defend his Olympic men’s singles title in Rio.
In a statement released by his management company, Murray said: “I’ve learned a lot from Amélie over the past two years. 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, 36, gave birth to her first child, Aaron, last August and took six months off from her coaching role, with Jonas Bjorkman covering for her. Bjorkman left Murray’s team at the end of 2015 when Mauresmo returned.
In a statement, Mauresmo, the former women’s world number one, said: “Working with Andy over the last two years has been a fantastic experience for me. 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 [his] team well and I hope he goes on to win many more titles.”
Although Murray failed to add to his haul of Grand Slam titles under her guidance, his performance as a clay court player improved.
The split comes less than two months after Murray, 28, dismissed talk of a rift between himself and Mauresmo as he adjusted to parenthood.
In March, Murray played down talks of problems with her after he crashed out of the Miami Open.
He told a post-match press conference: “If I’d had a falling out then Amélie wouldn’t be here at the tournament. We had dinner with all our families last night, so we certainly haven’t fallen out.”
Murray was the first leading male player to employ a female coach.
Speaking at the time of Mauresmo’s appointment, which followed his hugely successful relationship with Ivan Lendl, he said: “I’ve always had a strong female influence in my career and that’s something I needed right now.”