Talley's on-screen career began in 2002, with a minor part in the daytime soap opera As the World Turns. He appeared in three episodes of the drama series Summerland between June and July 2005 as Bryce. The following year, Talley made a guest appearance in the drama film Peaceful Warrior and on the sitcom Twins.
Talley was featured in Van Wilder: Freshman Year as the character Dirk Arnold and also starred as Eric P. Keller in the 2010 direct-to-DVD film Hole in One, which had various names prior to release. Recently Talley has moved on to less juvenile movies, landing the lead role of investigative reporter Matt Harper in Deadline, about the racially motivated murder of an African-America youth in the South. As well as film credits, Talley has also featured in a British television commercial for Pepsi Max. During Super Bowl XLIV, he drove a car in a Bridgestone commercial about a crazy bachelor party gone wrong. Talley is also featured in a 2010 Pizza Hut ad campaign. It was announced in late June 2012 that he would play Ella Montgomery's (Holly Marie Combs) love interest on Pretty Little Liars.