Arsenal women's head coach Jonas Eidevall resigned on Tuesday after three years at the club, following back-to-back defeats by Bayern Munich and Chelsea.
Assistant coach Renee Sledgers will take charge of the team on an interim basis, the Women's Super League club said in a statement.
Sixth-placed Arsenal have won only one of four league matches this season and lost 5-2 at Bayern in the Champions League last week before a 2-1 defeat by Chelsea.
"We thank Jonas for his commitment to the club and achievements here since joining us," Arsenal sporting director Edu Gaspar said in a statement.
Swede Eidevall, 41, won two Women's League Cup titles with Arsenal.
"Jonas has brought us back-to-back trophies... together with many memorable moments on the pitch," director of women's football Clare Wheatley said.