Wilshere had previously held the role of U18 coach at Arsenal before joining Norwich City a year ago. Upon Mehmet Ali's departure to Brentford, Wilshere was offered the U21 job at Arsenal.
Although Wilshere held talks with Arsenal's leaders about returning, he eventually decided against it. Wilshere's departure from Norwich City at the end of last season has left him available for other coaching opportunities.
Wilshere's next move is expected to be a senior post, as he looks to take on new challenges. Meanwhile, Max Porter and Ken Gillard have been in caretaker charge of Arsenal U21s during the preseason, with Porter now considered the favourite for the permanent position.