Troian Bellisario, Stana Katic, Jess Weixler and Michelle Trachtenberg are also on board.
The story revolves around four estranged sisters who reunite to mourn what they believe is the suicide of their mother.
Sean Hanish is directing and producing for Cannonball Prods. Lensing began last week in Los Angeles.
Paul Jaconi-Biery and Eleonore Dailly are producing “Sister Cities” with Hanish. Molina and CBS exec Kelly Kahl are exec producers.
Smart will next be seen in the independent comedy “Break Point,” opening in theaters on September 4. Recent credits include appearances on “Shameless” and “Justified.”
She is represented by Gersh and More-Medavoy.