He received wider recognition for his portrayal of musician Johnny Cash in the 2005 biographical film Walk the Line. His performance earned him several accolades and nominations, including the Golden Globe Award for Best Actor – Motion Picture Musical or Comedy and nominations for the Academy Award for Best Actor,Screen Actors Guild and BAFTA Award. He received his third Academy Award nomination for his critically acclaimed performance in the 2012 film The Master as well as his third nomination for a Golden Globe Award and BAFTA Award. In 2013, he received his fourth nomination for the Golden Globe Award in the category Best Actor – Motion Picture Musical or Comedy, for his role as Theodore Twombly in Spike Jonze's film Her.
Aside from his acting career, he has also ventured into directing music videos, as well as producing films and television shows. He has recorded an album, the soundtrack to Walk the Line, for which he won a Grammy Award.