Baccarin landed her first movie role in the improvised fashion world comedy Perfume (2001). This was followed by a lead role in the film festival hit Way Off Broadway (2001). Baccarin appeared with Natalie Portman and understudied for her role in the acclaimed Central Park production of The Seagull. The science-fiction drama Firefly was Baccarin's first television series, and she reprised her role of Inara Serra in the 2005 film Serenity.
In February 2005, Baccarin provided the voice for Black Canary in multiple episodes of the animated series Justice League Unlimited. She also guest starred in three episodes of the television series The O.C. in 2006. Morena also acted in an unaired pilot episode of It's Always Sunny in Philadelphia, playing Carmen, a male-to-female transsexual.
It was announced in April 2006 that Morena would be playing the adult version of Adria, a recurring villain in the tenth season of Stargate SG-1. She first appeared in season 10 episode "Counterstrike" as adult Adria (the younger versions of Adria were previously played by other actresses). Morena reprised her role as Adria in the movie Stargate: The Ark of Truth.
In May 2009, Baccarin made her off-Broadway debut in Theresa Rebeck's television satire Our House at Playwrights Horizons in New York City.
Baccarin landed the lead role of Anna, the leader of the alien Visitors, in ABC's 2009–2011 series V, a remake of the 1984 series. In May 2011, shortly following the airing of the show's second season finale, it was announced that the show would not return for a third season.
That same month, Baccarin joined the cast of the Showtime television drama Homeland, for which she won acclaim for her performance as the conflicted wife of a former prisoner of war.
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