The only French side in Super League had lost their last five matches in a row including the 18-10 late defeat by Huddersfield at Magic Weekend.
Frayssinous, 40, is a former Catalans and France stand-off who became the first French coach of the club when he replaced Trent Robinson in 2012.
Coaches Jerome Guisset and Michael Monaghan and general manager Alex Chan will take charge of the first team.
Catalans Dragons have parted company with head coach Laurent Frayssinous.