From 2012 to 2013, Buckley starred in the short-lived horror drama series "666 Park Avenue", portraying struggling playwright Brian Leonard who moves into a haunted building with his wife. In 2013, he was cast in a two-episode guest arc on season three of The CW's comedy-drama series "Hart of Dixie". The following year, he co-starred in the "Veronica Mars" web spin-off series "Play It Again, Dick", featuring Ryan Hansen in the central role. In 2015, he began starring as Major Lilywhite on The CW's comedy-drama horror series "iZombie". In June 2016, Buckley was cast to star in the first episode of the Hulu anthology series "Dimension 404", alongside Lea Michele and Joel McHale.