Brown made his first appearance of the season in the Steelers' season-opener against the Baltimore Ravens and finished with two receptions for 14 yards and had three kickoff returns for 34 yards in a 35–7 loss. On October 30, 2011, Brown had a season-high nine receptions for 67 yards and caught his first career touchdown reception on a seven-yard pass from Ben Roethlisberger in a 25–17 victory over the New England Patriots. The next game, he caught five passes for 109 yards, marking his first career game with over 100 receiving yards, in a 23–20 loss to the Baltimore Ravens. On November 13, 2011, he earned his first career start and made five receptions for 86 yards in a 24–17 defeat of the Cincinnati Bengals. On December 4, 2011, he returned a punt for a 60-yard touchdown and made two catches for 67 yards, as the Steelers routed the Cincinnati Bengals 35–7. The punt return for a touchdown was the first in his career and Brown was named AFC Special Teams Player of the Week for his performance. In a Week 14 win over the Cleveland Browns, he made his second start of the season and ended the game with five catches for a season-high 151-yards and scored a season-long 79-yard touchdown in a 14–3 victory. He finished the season with 69 receptions for 1,108 yards and two touchdown receptions in 16 games and three starts. The Pittsburgh Steelers finished 12–4 and received a playoff berth. On January 8, 2012, Brown caught five passes for 70 yards and had one carry for 18 yards in a 29–23 overtime loss to the Denver Broncos in the AFC Wild Card Round.