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The following year, her ability to look like a wide-eyed Disney animated heroine helped her to be chosen from about 300 actresses auditioning for the role of Giselle in the animated/live-action feature film Enchanted which would prove to be her major break-through role. Her vivacious yet innocent portrayal allowed her to use her singing and dancing talents. Her performance garnered a Golden Globe Award nomination for Best Actress in a Motion Picture Musical or Comedy.
Adams next appeared in the major production Charlie Wilson's War and went on to act in the independent film Sunshine Cleaning which premiered at the 2008 Sundance Film Festival.
In 2008, she also starred as Delysia Lafosse in Miss Pettigrew Lives for a Day. She sings "If I Didn't Care" in the film.
Next, her portrayal of Sister James in Doubt which brought her a second Academy Award nomination for Best Supporting Actress as well as nominations for a Golden Globe, a Screen Actors Guild award, and a British Academy Film award.
She next appeared as Amelia Earhart in Night at the Museum: Battle of the Smithsonian and as a post-9/11 hot line counselor, aspiring writer, amateur cook and blogger in Julie & Julia.
In March 2008, Adams hosted the seventh episode of the 33rd season of Saturday Night Live. In the episode, she played various characters, and sang "What is this Feeling" from Wicked in a mock battle with SNL cast member Kristen Wiig during the opening monologue.
In 2010 she stared as Charlene Fleming in The Fighter. For this role, Adams was nominated for the Golden Globe Award, Broadcast Film Critics Association Award, a BAFTA Award, and a Screen Actors Guild Award for Best Supporting Actress.