Murray slips in rankings and splits with Mauresmo
Murray, 28, said he had “learnt a lot” from two-times Grand Slam champion but “time and travel had been a challenge”.
They “mutually agreed” to end the partnership which began in June 2014.
Since then, Murray has won seven titles, but failed to build on the two Slams – US and Wimbledon – that he won under Ivan Lendl.
In a joint statement, Murray said: “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.”
Mauresmo, 36, added: “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. I wish him and the team well and I hope he goes on to win many more titles.”
Murray lost his number two ranking to Roger Federer after losing the Madrid Open final in three sets to old foe Novak Djokovic.
Murray, defending champion, had seven opportunities to break his opponent in the final game which lasted 14 minutes.
But the world number one clung on to secure his 29th Masters title 6-2, 3-6, 6-3.
The Scot struggled in the opening set but fought back to take the second. Djokovic has moved ahead of Rafael Nadal with a record 29 ATP Masters 1000 titles.
Despite losing, his performances on the clay courts will boost Murray’s chances of progressing at the French Open which begins on 22 May.