The pair joined forces on New Year's Eve in 2011 and since then Murray has ended his wait for a Grand Slam title by winning the US Open and Wimbledon, as well as claiming a gold medal at the Olympic Games in London.
However, having achieved that success, Lendl believes that the time is right for the two to go their separate ways.
"Working with Andy over the last two years has been a fantastic experience for me. 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," said the eight-time Grand Slam champion.
"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."
Meanwhile, world number six Murray added: "I'm eternally grateful to Ivan for all his hard work over the past two years, the most successful of my career so far. 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."