Smith appeared in 8 games as a true freshman in 2011 season, recording a forced fumble in a 31–3 win over Ole Miss in the Egg Bowl. In 2012, Smith appeared in all 13 games and led the Bulldogs with 4.5 sacks. As a junior in 2013, Smith recorded 2.5 sacks, including 2.0 in a 59–26 loss to LSU. Smith started the 2014 season with a bang, winning the SEC Defensive Lineman of the Week Award in each of the first three weeks. Smith recorded an interception in the Bulldogs' 49–0 rout of Southern Miss, and returned another acrobatic, one-handed interception for a touchdown in the Bulldogs' win over UAB. Smith ended the season with 42 tackles, nine sacks, two interceptions and a touchdown. At the end of his senior season, Smith was projected as a fourth-round pick in the 2015 NFL Draft by CBS and NFL Draft Scout.
Professional career
Washington Redskins
The Washington Redskins selected Smith in the second round of the 2015 NFL Draft. Smith was the seventh defensive end drafted in 2015.
2015
On May 11, 2015, the Washington Redskins signed Smith to a four-year, $5.77 million contract that includes $3.16 million guaranteed and a signing bonus of $2.46 million. Throughout training camp, Smith competed to be the backup right outside linebacker against veteran Trent Murphy. Head coachJay Gruden named Smith the backup right outside linebacker to start the regular season, behind Murphy, after Junior Galette sustained a season-ending injury. He made his professional regular season debut in the Washington Redskins’ season-opener against the Miami Dolphins and made two solo tackles, forced two fumbles, a fumble recovery, and made his first career sack as they lost 17-10. During the third quarter, Smith recovered a fumble he caused while making his first career sack on quarterback Ryan Tannehill for a 13-yard loss. In Week 13, Smith earned his first career start and recorded one solo tackle as the Redskins earned a 24-21 victory at the Chicago Bears. On December 26, 2015, Smith tied his season-high of four combined tackles and also had a season-high three sacks on Sam Bradford during a 38-24 victory at the Philadelphia Eagles in Week 16. His performance earned him the Pepsi NFL Rookie of the Week. He finished his rookie campaign with 35 combined tackles, eight sacks, four pass deflections, three forced fumbles, and a fumble recovery in 16 games and one start. The Washington Redskins finished first in the NFC East with a 9-7 record and clinched a playoff berth. On January 10, 2016, Smith appeared in his first career playoff game and recorded three combined tackles, a sack, and earned the first safety during a 35-18 loss against the Green Bay Packers in the NFC Wildcard Game.
2016
In March 2016, Smith was voted as one of the best under-25 players in the NFL. Smith entered training camp slated as a backup outside linebacker behind Junior Galette and Ryan Kerrigan. Head coach Jay Gruden named Smith the starting right outside linebacker after Junior Galette sustained a torn Achilles during the 2016 preseason. In a game against the Minnesota Vikings in November 2016, Smith had two sacks, along with his first career interception, helping the Redskins to a 26–20 win.
Smith had a strong performance in the 2017 win against the Arizona Cardinals recording a sack, his second career interception, and a fumble recovery caused by Anthony Lanier. In the last game of the season, Smith recorded his third career interception on New York Giants quarterback Eli Manning. At the end of the 2017, he tied his season-high of eight sacks.
In 2018, Smith recovered a fumble caused by Ryan Kerrigan in the end zone helping to seal the Week 7 win against the Dallas Cowboys and recording his first career touchdown. Smith recorded his fourth career interception against Houston Texans quarterback Deshaun Watson in Week 11.
Green Bay Packers
2019
On March 14, 2019, Smith signed with the Green Bay Packers on a four-year, $52 million contract. In Smith's debut as a Packer in Week 1 against the Chicago Bears, he made 5 tackles and sacked Mitchell Trubisky 1.5 times in the 10–3 win. In Week 3 against the Denver Broncos, Smith sacked Joe Flacco 3 times and forced a fumble that was recovered by the Packers in the 27–16 win, earning him NFC Defensive Player of the Week honors. In week 6 against the Detroit Lions, Smith sacked Matthew Stafford 1.5 times in the 23–22 win. In week 10 against the Carolina Panthers, Smith recorded 2 sacks on Kyle Allen in the 24–16 win. In Week 16 against the Vikings, Smith recorded 3 tackles and 1.5 sacks during the 23-10 win. In the Divisional Round of the playoffs against the Seattle Seahawks, he recorded 2 sacks on Russell Wilson during the 28–23 win, including one at the 2 minute warning in the 4th quarter. He finished the season with 56 tackles, 12 sacks and four pass deflections.