[10] Schmidt moved to New York City to intern with an off-Broadway theatre company, and worked three jobs as she began auditioning for acting roles.

[13] She served as an understudy in a national tour of Edward Albee's Who's Afraid of Virginia Woolf?, starring Bill Irwin and Kathleen Turner, directed by Anthony Page.

[11][12] She appeared in the title role of Sive at the Irish Repertory Theatre in 2007, and was then an understudy in a revival of Come Back, Little Sheba on Broadway.

[15][16][17] Schmidt made her film debut in the 2010 documentary Client 9: The Rise and Fall of Eliot Spitzer, portraying a prostitute who refused to appear on camera.

She was also cast in the play Be a Good Little Widow at Ars Nova, and in Teresa Deevy's Temporal Powers at Manhattan's Mint Theater in 2011.

[28] Schmidt stars in Apple TV+ original series For All Mankind (2019–present), which explores an alternate history where the Soviet Union reaches the moon before the United States, leading to the Space Race continuing far beyond its historical end, playing the central role of NASA engineer Margo Madison.