Jones started his junior season with a solid performance against San Diego State with six receptions for 93 yards and a touchdown in the 48–3 victory. Two weeks later, Jones had five receptions for 106 yards and a touchdown in a 62–13 victory over Duke. On October 9, in a conference game against #19 South Carolina, Jones had eight receptions for 118 yards and a touchdown in the Crimson Tide's 35–21 loss to the Gamecocks. On October 23, Jones torched the Tennessee Volunteers for 221 yards on 12 receptions, which were good for collegiate career highs in both, in a 41–10 victory at Neyland Stadium in Knoxville, Tennessee. On November 6, Jones had 10 receptions for 89 yards and a touchdown in a 24–21 loss to #12 LSU at Tiger Stadium in Baton Rouge, Louisiana. One week later, Jones was held to only three receptions for 41 yards in a 30–10 victory over Mississippi State but had a 56-yard rushing touchdown in the victory. In the following game, against Georgia State, he recorded his first collegiate game with two receiving touchdowns in the 63–7 victory. On November 26, in the Iron Bowl against #2 Auburn, Jones had ten receptions for 199 yards and a touchdown, but the Crimson Tide lost to the Tigers by a score of 28–27. The Crimson Tide reached a bowl game, which was Jones's final collegiate game. In the 2011 Capital One Bowl against Michigan State, Jones had three receptions for 49 yards and 36 rushing yards and a rushing touchdown in the 49–7 victory.
On January 7, 2011, Jones decided to forego his senior season of college football. Instead, he chose to declare eligibility for the NFL Draft with teammates Mark Ingram, Greg McElroy, and Marcell Dareus. Jones was later invited to the "All-Star Football Challenge", a skill contest shown by ESPN on February 4. He excelled at the 2011 NFL Combine, posting the longest long jump and the third fastest 40-yard dash among wide receivers, despite having a broken bone in his foot.
The Atlanta Falcons selected Jones with the sixth overall pick of the 2011 NFL Draft. Atlanta traded five draft picks to the Cleveland Browns to move up into their spot and take Jones, giving up their 27th, 59th, and 124th picks from the 2011 Draft, and their first and fourth round picks from the 2012 Draft. He was the second wide receiver to be taken in the 2011 NFL Draft, behind only A. J. Green of the Georgia Bulldogs, who was selected fourth overall by the Cincinnati Bengals. In addition, he was one of five Alabama Crimson Tide players to be selected that year. Jones wears #11 with the Falcons.
Jones came to terms with the Atlanta Falcons on July 28, 2011, signing a four-year contract worth $16.2 million, all of which was guaranteed. His NFL debut came against the Chicago Bears at Soldier Field. In the 30–12 loss, he had five receptions for 71 yards. In Week 4, against the Seattle Seahawks, he had 11 receptions for 127 yards in the 30–28 victory for his first game going over the century mark. He recorded his first two NFL touchdowns on Week 9 of the 2011 season, against the Indianapolis Colts in a 31–7 victory. Jones's first touchdown was a 50-yard reception from quarterback Matt Ryan in the first quarter, and the second touchdown was an 80-yard reception from Ryan in the second quarter. After having quiet games against the New Orleans Saints and the Minnesota Vikings, Jones bounced back against the Houston Texans with four receptions for 68 yards in the 17–10 loss. Jones finished his rookie season strong by combining for 393 receiving yards and six touchdowns over the last four games of the regular season. He finished the season leading all rookies in touchdown receptions with eight, while his 54 receptions for 959 yards ranked him second among rookies in yards and touchdowns, behind A. J. Green, of the Cincinnati Bengals and third in catches behind Green and Greg Little, of the Cleveland Browns. He was named to the NFL All-Rookie Team for the 2011 season.