Aidy Boothroyd is to leave his role as England U21 head coach with immediate effect after five years in charge.
The former Watford manager's contract is up in the summer, but he has decided to call time early following the team's elimination from the European Championships.
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.
Boothroyd had described the job as "utterly impossible" during last month's group stages of the European Championships, claiming the primary aim of the U21s is to get players to Gareth Southgate's senior squad.
Jude Bellingham, Reece James, Phil Foden and Mason Mount were among the players who could have been included in the squad in Slovenia, but instead featured for the senior team's World Cup Qualifiers.
"My job isn't to say to Gareth we should have Jude, Phil or Mason, it is about the senior team and it always will be," Boothroyd said.
The Young Lions began their U21 Euros campaign with defeats to Portugal and Switzerland in the group stages.
Their hopes of reaching the quarter-finals were then dashed in the final minutes against Croatia, with a 2-1 victory not enough for Boothroyd's side to progress as Domagoj Bradaric's injury-time stunner proved crucial.
Boothroyd, who replaced Southgate in the role in 2016, had enjoyed an unbeaten qualifying campaign with the U21s to reach the tournament.
He had also overseen their previous two European Championships, with England reaching the semi-finals in 2017 before crashing out of the groups in 2019.
England last won the U21 Euros in 1984, while the 2021 group-stage exit was their fifth in the past six editions.
In 2018, Boothroyd steered England to a third successive Toulon Tournament title, with the 2-1 victory over Mexico in the final emulating the achievements of Southgate's U21s in 2016 and Neil Dewsnip's mixed-age group a year later.
'If U21s not about success, don't enter tournaments'
Sky Sports' Andy Hinchcliffe, who covered all three of England's games at this year's U21 tournament, said there was little point in entering international competitions without an aim to build a winning mentality among younger age groups.
He said: "Of course it's about progression, but why enter a tournament if you think winning games, or the tournament, breeding a winning mentality, doesn't matter? That has to be as important as being a pathway to the senior England team.
"Darren Bent was talking about how getting into the seniors is more about how you play for your clubs than for the England U21s.
"If the message for the U21s is about style, how we play the game, your development as an international and not about how we win games, getting a winning mentality, then going to tournaments is absolutely pointless. We might as well play a load of U21 friendlies if it's about how you play rather than the results.
"You look at Spain, Italy, Portugal, Germany, they breed winners. That's the point of going to tournaments, working out how to get the job done in tournament football. It's not the same as qualifying, you're together for a longer period of time, you're against better opposition. It's about how you get the job done, then you can take that down the line into senior England competitions.
"Yes, the squad could've been better with Jude Bellingham, Phil Foden and Trent Alexander-Arnold in it, but we've had very good squads in the past and they've not been able to get out of the group stages.
"It's starting to be a historic problem, and if it is about a pathway rather than being successful, then don't enter tournaments, because it's a waste of time - because we're not learning anything about how to progress at this level of tournament football.
"Breeding a winning mentality isn't just about winning with style, it's about winning when you're not the better team. Have you got the experience, have you got the experience of winning when you're not the best team?
"That's where England fell short in two of these games. In three matches, if you're not the better team, you're Gareth Southgate looking at that and thinking that has to be a bit of a worry."