Wayne Rooney and Plymouth have “mutually agreed to part ways with immediate effect” after a nine-game winless run.
Rooney, 39, leaves with the club sat bottom of the Sky Bet Championship, four points from safety.
“We would like to thank Wayne and his team for all their efforts and wish them well for the future,” a statement said.
Following Rooney’s departure, first-team coach Kevin Nancekivell and club captain Joe Edwards will be in charge for Plymouth’s New Year’s Day clash against Bristol City.
Also departing the club will be assistant head coach Mike Phelan and first team coach Simon Ireland, the team said.
In a statement on the Plymouth website, Rooney thanked those who are on the board as well as the staff, players and fans.
“Thanks to all the staff who made me feel welcome and who make the club such a special place, the players and fans for their efforts and support during my time as head coach and I wish them all the best for the future,” he said.
“To the Green Army thanks for making the games at Home Park so special, they are memories that we will share forever.
“I would also like to give a special mention to my coaching staff Kevin Nancekivell, Simon Ireland, Darryl Flahavan and Mike Phelan for their knowledge, dedication, help and support.
“Plymouth Argyle will always hold a special place in my heart, and I will continue to look out for and take interest in their results.”
Rooney replaced Ian Foster in May on a three-year deal at Plymouth. He managed to oversee 23 Championship games, racking up four wins, 13 defeats and six draws.
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The former Manchester United and England forward’s last game at the helm came on Sunday, when Argyle were beaten 2-0 at fellow strugglers Oxford.
It marks the second setback for Rooney in 2024 following his dismissal as Birmingham City head coach in January.
He has previously managed Derby County and Major League Soccer (MLS) side DC United.