In 2011, he joined the cast of the Australian police drama On the Edge, playing Staff Sergeant Charlie Lewis. In 2013, he received a leading role in the American TV series Banshee. Anthony Starr played the role of Lucas Hood, a former prisoner and professional thief who assumed the identity of the sheriff of the Banshee (town in Pennsylvania).

Since 2019, he has starred in the TV series The Boys as Homelander.