The British number one made the announcement on his official website on Wednesday in a move which will cause some surprise.
Murray was always a player of huge promise but only made the step up to a grand slam champion under the coaching of Lendl, himself an eight-time major winner who, like Murray, lost his early slam finals.
Success for the duo first came at the London Olympics before a real breakthrough in winning the 2012 US Open. Their greatest glory together, though, was last year's Wimbledon, at which Murray ended a 77-year wait for a male British champion.
Murray, who is returning from back surgery and preparing to defend his title in Miami, said: "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."
Lendl added: "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.
"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."
Murray, 26, appointed Lendl as his coach on December 31, 2011 after working with a number of others.
The likes of Leon Smith, Mark Petchey, Brad Gilbert, Miles Maclagan and Alex Corretja had all sat in his corner, but linking up Lendl was seen as a shrewd move.
Like Murray, Lendl lost his first four grand slam finals before going on to top-level glory and results dictated that their partnership was working well.
"He's made me learn more from the losses than I did before and he's always been very honest with me and believed in me when other people maybe didn't," Murray said of the 54-year-old Czech in the wake of his Wimbledon win.
"Ivan's been very patient, as I'm not always easy to deal with. He's also honest with me. If I work hard he's happy, if I don't he's disappointed and he'll tell me. He has got me mentally slightly different going into these big matches."
The split will take many by surprise, although there has been a downturn in Murray's results since Wimbledon. That, though, can largely be attributed to the back injury he had and the surgery he has since undergone.