
During his first season with the Steelers, the team advanced to Super Bowl XLV but lost to the Green Bay Packers. He finished his rookie season with 16 receptions for 167 yards in ten games. During his second season, Brown became the first player in NFL history to have more than 1,000 yards receiving and returning in the same year. For his efforts, Brown was selected as a punt returner for the 2012 Pro Bowl. In 2013, Brown became the only receiver in NFL history to record five receptions and at least 50 yards in every single game of an NFL season. Although his on-the-field productivity continued over the next several seasons, including leading the league in receiving yards in 2014 and 2017, Brown's relationship with the Steelers worsened, especially with quarterback Ben Roethlisberger.
In 2019, he was traded to the Oakland Raiders, who then made him the highest-paid receiver in the league. However, his time in Oakland was short-lived, and following several off-the-field incidents, including a confrontation with general manager Mike Mayock, the team released Brown without him ever playing a regular season game. Brown signed with the New England Patriots shortly thereafter, but was cut after appearing in only one game. At the time, the NFL was investigating allegations of sexual assault against Brown.