On November 24, 2013, Smith reportedly agreed to a three-year contract for $15 million with the Los Angeles Angels of Anaheim, pending the completion of a physical. On November 27, 2013, the Angels confirmed that the team and Smith agreed to the terms. On April 25, 2014, Smith was named the Angels' new closer after multiple struggles by former closer Ernesto Frieri. After the Angels traded for San Diego Padres' All-Star closer Huston Street on July 18, 2014, Smith was moved to an eighth-inning setup role. Smith finished with 15 saves in 76 games to the tune of a 1.81 ERA.