Andrew Altman will leave the corporation on 15 August after three years in the role.
As head of the corporation – which includes the former Olympic Park Legacy Company – Altman has led plans to transform the 500-acre Olympic Park into an events destination as well as working on other developments like housing and regeneration.
The LLDC said the park's legacy was now secure and the next development phase would be one of constructing new venues after the Games, such as a museum for the park.
The recruitment process has begun for Altman's successor. Dennis Hone, chief executive of the Olympic Delivery Authority will act as a part-time interim chief executive in the meantime.
During his tenure, Altman secured post-Games operators for major venues including the Aquatics Centre, Multi-use Arena and Orbit as well as securing over £400 million for infrastructure, programming and regeneration.
He said: "It has been a tremendous honour to lead this once-in-a-lifetime project that will transform the face of London and will be a spectacular example of city-building the world over.
"I am proud to have been able to set the table with a clear vision, resources and commercial investment. It is now the perfect time to transition the project to one focused on construction, so there will no disruption after the Games in implementing the legacy vision we have crafted."
Daniel Moylan, the incoming chairman of the LLDC said: "Andy Altman has made a huge personal contribution to the future of the Olympic Park and we thank him for putting us in such a strong position."
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