The Swede has played a key role under Mikel Arteta - but the former Gunners player has taken the decision to leave the club to further his coaching career.
Ljungberg has held various positions at the club, including interim head coach following the departure of Unai Emery.
But the club icon will now continue his career away from the Emirates.
Confirming his departure on Twitter, Ljungberg said he was grateful to the club for giving him a chance to develop as a coach but now wants to step up his attempts to become a manager.
'I have decided to leave my first team assistant coaching role at @Arsenal to progress my management experience,' he wrote. 'I have been involved with this club on and off since 1998 and am grateful for all the opportunities they have given me both as a player and as a coach.
'I wish Mikel and all the team every success for the season ahead. Thanks also to the fans for their constant support and for always being by my side. I hope we will all meet again soon.
The 43-year-old played for Arsenal for nine seasons between 1998 and 2007 - making 325 appearances. He went on to play for West Ham and Seattle Sounders before retiring and joining Arsenal as an ambassador in 2013.
Three years later he became part of the set-up at their academy to coach the Under-15s. He had a short spell as Wolfsburg's assistant manager in 2017 before returning to Arsenal the following year - this time taking charge of the U-23s.
In 2019 he was promoted to Emery's first team coaching group before being picked to lead the senior squad on a caretaker basis.
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