The Baltimore Ravens selected Smith in the 2nd Round (58th overall) of the 2011 NFL Draft. Smith started out slow in the preseason and struggled with drops. However, in Week 3 against the St. Louis Rams, Smith had five catches for 152 yards and three touchdowns. His first catch in the NFL was a 74-yard score from quarterback Joe Flacco. Smith continued his good play, even catching a game-winning touchdown against the Pittsburgh Steelers at Heinz Field on November 6, 2011. Smith finished his first season with 50 catches for 841 yards and seven touchdowns.