Aidy Boothroyd will vacate his role as manager of the England U21s with immediate effect after five years in charge.
Boothroyd’s contract was up this summer but he has decided to step down from the role following England’s exit from the European Championships.
England were eliminated from the group stages of the tournament after losing two of their three matches last month.
A last-gasp goal from Croatia in England's 2-1 win meant they just missed out on a place in May’s quarter-finals.
We can confirm that #YoungLions coach Aidy Boothroyd is to depart the @FA after a seven-year spell with the organisation:
— England (@England) April 16, 2021
Boothroyd said: "It's been the greatest privilege to represent the FA and lead England teams into high-profile tournaments.
"While we didn’t finish in the way we wanted, I'm very proud to have been able to work so closely with players who I know will go on to have remarkable international careers and to have experienced some very special moments with them over the years.
"I'd like to thank my staff and all of the incredible support team that have done so much to help us remain competitive against other elite nations.
"In every single get-together they embraced our unique challenge of rightly prioritising the needs of the senior team while ensuring we gave our all to try and get a positive performance and result."
England senior boss Gareth Southgate added: "I’d like to thank Aidy for his wholehearted support and dedication to developing English players and coaches across the last seven years.
"His pride in working with all of our development teams has shone through and his support of the senior team has been greatly appreciated. I wish him every success on the next step of his career."
The FA will now begin a recruitment process for Boothroyd's replacement, while it is thought the 50-year-old wants a return to club management.