His big break came in the 2008 film The Boy in the Striped Pyjamas. Director Mark Herman said that they came across Butterfield early on in the audition process. He was on the first audition tape he received and he was the third hopeful he met in person. Herman thought Butterfield's performance was amazing, but only decided to cast him after auditioning hundreds of other boys.

Also for 2008 he landed a role in an episode of Merlin (The Beginning of the End) he played a young druid boy who is hunted by Uther Pendragon who wants to sentence him to death because he feels threatened by the boy's magic. Butterfield has stated in a TimesOnline interview “I don’t really want to be an actor,” but nonetheless has snagged roles such as in Nanny McPhee and the Big Bang and The Wolfman both in 2010. He also plays the role of 'Hugo' in Hugo (2011) and has landed the role of "Ender Wiggin" in Ender's Game (2013).

He's already been nominated for several awards. He was nominated in the category "Most Promising Newcomer" of the British Independent Film Awards, but he was beaten by Dev Patel from Slumdog Millionaire. He has also been nominated for the NSPCC Award (Young British Performer of the Year) in the London Critics Circle Film Awards. And a Young Artist Award Nomination for Best Performance in an International Feature Film - Leading Young Performers.