Balaban made a successful follow-up with Saint Jude (2000), directed by John L'Ecuyer. She starred in the TV movie After the Harvest (2001), opposite Sam Shepard, and appeared in Happy Here and Now (2002), opposite David Arquette and Ally Sheedy. She also starred in the horror film Spliced (2002), co-starring Ron Silver. Balaban was a member of the garage/electro/pop band We are Molecules where she sang and played keyboards and drums. She has also written for arts newspapers.
While previously unsure of acting as a career, Balaban committed to seriously pursuing acting around 2007. She appeared in her first mainstream Hollywood feature film, Definitely, Maybe in 2008, a romantic comedy starring Ryan Reynolds. She next appeared in Last Chance Harvey, a romance starring Dustin Hoffman and Emma Thompson which had a wide release in January 2009. She plays the supporting role of Susan, the estranged and soon-to-be-married daughter of Hoffman's character. She described her time in London making the film as "going to the best acting school in the world" to The Globe and Mail.
Balaban starred in the independent drama One Week (2008), directed by Michael McGowan. She played Samantha Pierce, whose fiancé (Joshua Jackson), is diagnosed with terminal cancer and takes a motorcycle trip across Canada. She was nominated for the Genie Award for Best Performance by an Actress in a Supporting Role in 2010 for her performance. Balaban starred in the black comedy You Might as Well Live in 2009, playing a psychotic girl who is obsessed with explosives. She appeared in the 12 minute short film "Goblin Market", directed by Adam Leith Gollner, which was presented at the 2009 Pop Montreal festival. As of 2009, Balaban was also trying to write her own screenplay and doing improvisational theatre in Montreal.
Balaban's other films in 2009 include Not Since You, a drama about a group of college friends, and The Trotsky, by Jacob Tierney. She also shot the CBC TV movie Abroad, based on the love life of Leah McLaren, a Toronto columnist for The Globe and Mail. Balaban was nominated for the Gemini Award for best lead actress in a dramatic program or miniseries for the role. She starred in "The New Tenants" with Vincent D’Onofrio, a short film entered into the CFC Worldwide Short Film Festival.
Balaban starred in the 2010 comedy/drama Coach, directed by Will Frears, as an emergency room doctor who falls for an inner city soccer coach (Hugh Dancy). Balaban will appear as a journalist opposite Paul Ahmarani in The Future is Now!, a film that combines elements of documentary and drama by Gary Burns. She appears in the episode "Communication Breakdown" of the TV series Covert Affairs playing Natasha Petrova, a Russian computer hacker, and the character Auggie (Chris Gorham)'s ex-girlfriend.
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