According to Entertainment Weekly, Simpson-Wentz will have a role in the series being brought back to TV by the CW network.
The 24-year-old singer will play Violet, a young woman from a small town, who looks naive, but is really a calculating manipulator.
Simpson-Wentz joins Katie Cassidy and Michael Rady in the cast.
Last March, the young singer and her husband, Pete Wentz, guest starred on the series CSI: NY, playing characters inspired by Bonnie and Clyde.