Gordon-Levitt shared his excitement Wednesday on Twitter about snagging the four-time Oscar nominee for his turn behind the camera.
Moore joins Scarlett Johansson in the film. In addition to handling directing chores, Gordon-Levitt will star a swinging Don Juan type who tries to mend his ways.
Shooting is scheduled to start in April.
Moore recently earned favorable reviews for her portrayal of Sarah Palin in HBO's "Game Change."
Variety first reported Moore's casting.