De Pauw leaves Villa in ninth-place in the Women's Super League after collecting just six points from their opening nine games.
Villa have won just one league game under de Pauw this season and Sunday's 4-0 defeat against Arsenal left them just one-point above the relegation zone.
The Dutchman, who previously managed FC Twente and Bayer Leverkusen, was appointed as manager in June after Carla Ward stepped down from her role at the end of last season.
"We would like to thank Robert for his commitment during his time in charge and wish him well for the future," Villa said in a statement.
Assistant head coach Shaun Goater has been placed in interim charge while Villa continue their search for a new manager.