She appeared in the 2010 comedy film Get Him to the Greek, starring Russell Brand and Jonah Hill, and she was co-lead in the James Wan horror film Insidious, which premiered in September 2010 at the Toronto International Film Festival In 2013, Byrne appeared in the crime drama The Place Beyond the Pines, with Ryan Gosling and Bradley Cooper, and appeared in the comedy, The Internship, opposite Vince Vaughn and Owen Wilson; and The Turning, a short film installment in a Tim Winton omnibus feature.
Byrne also played the newlywed wife in I Give It a Year, a comedy about the trials and tribulations of a couple during their first year of marriage.
In 2009, Byrne co-starred with Nicolas Cage in the science fiction thriller Knowing.
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Byrne was in a relationship with Australian writer, director and actor Brendan Cowell for over six years.
Cowell moved from Sydney to New York City, following Byrne's success on Damages. As of 2013, Byrne lived in New York and said she remains insecure about a stable career: "I don't think that insecurity ever leaves you.
Byrne admitted that "watching myself is confronting because I'm convinced I can't act and I want to get out, that's how insecure I am." Byrne appeared as a guest in an episode of the police drama series Murder Call.
On stage, she played a lead role in La Dispute and in a production of Anton Chekhov's classic Three Sisters at the Sydney Theatre Company.
In 2003, she starred in three Australian films: The Night We Called It a Day with Melanie Griffith and Dennis Hopper; The Rage in Placid Lake for which she was named Best Actress at the Australian Film Institute; and Take Away, another comedy.