She is known for her role as Lindsay on You"re the Worst and her role as a capella leader Alice in Pitch Perfect. In January 2016, Donohue appeared in the role of January in the Fox presentation of Grease Live. She is best known for the voice of the temperamental divaesque Lily on the Nicktoons Network "anime" series Kappa Mikey, Angela Rains on 5D"s, and Zoe and Chomp on Dinosaur King.
Donohue was also featured in the video for "Coder Girl" by Dale Chase.
She studied at the Anthony Meindl Acting Center.