Murray and Lendl announced their decision on the British player's blog on Wednesday, a few days after Murray lost in the fourth round at Indian Wells.
"I'm eternally grateful to Ivan for all his hard work over the past two years, the most successful of my career so far," said Murray, who returned from back surgery this season. "As a team, we've learned a lot and it will definitely be of benefit in the future. I'll take some time with the team to consider the next steps and how we progress from here."
With Lendl, Murray won Olympic gold in London in 2012 and the U.S. Open title later the same year. In 2013, he became the first British man to triumph at Wimbledon in 77 years.
Before winning the U.S. Open, Murray was 0-4 in Grand Slam finals. Only one other man in the Open era, which began in 1968, lost his first four major titles matches: Lendl. The Czech-born baseline player then went on to win eight Grand Slam singles titles during a 17-year career, spending 270 weeks at No. 1 in the world rankings.
Lendl first got involved with Murray in December 2011. Despite a lack of coaching experience, Lendl immediately struck a chord with his protege as Murray made it to the Wimbledon final, where he lost to Roger Federer in four sets.
Murray's breakthrough came a month later when he beat Federer in the Olympic final at the All England Club. He then defeated defending champion Novak Djokovic in the final at Flushing Meadows to win his first Grand Slam singles title.
"Working with Andy over the last two years has been a fantastic experience for me," Lendl said. "He is a first class guy. Having helped him achieve his goal of winning major titles, I feel like it is time for me to concentrate on some of my own projects moving forward including playing more events around the world which I am really enjoying.
"I will always be in Andy's corner and wish him nothing but great success as he too goes into a new phase of his career."
Lendl has recently played exhibitions in Kansas City, Oklahoma City, Nashville, Charlotte and London. He has also been giving clinics in the Canary Islands as well as opening new courts in Bluffton, South Carolina, at the Ivan Lendl Junior Tennis Academy.
Murray will be defending his Miami title next week before leading Britain in the quarterfinals of the Davis Cup next month against Italy.