As a true freshman at Alabama in 2015, Payne had 13 tackles and half a sack.[3] As a sophomore in 2016, he had 36 tackles and 1.5 sacks.[4][5] In the National Championship Game against Clemson, he recorded five tackles and a half sack.[6]
As a junior in 2017, Payne was named the defensive MVP of both postseason games that Alabama played.[7][8] In the Sugar Bowl versus Clemson, he intercepted a ball and scored an offensive receiving touchdown on the resulting drive. In the National Championship Game against Georgia, Payne had six tackles to help lead Alabama to their second national championship in three seasons.[9] After his junior year, Payne declared his intentions to enter the 2018 NFL draft.[9] During his time at Alabama, Payne's given name was commonly misspelled as Da'Ron, which he requested to change back to Daron for his professional career.[10][11]
Payne was selected by the Washington Redskins in the first round (13th overall) of the 2018 NFL draft.[14][15] On May 10, 2018, Payne signed a four-year contract worth US$14.4 million featuring a $8.56 million signing bonus.[16] He recorded his first career sack in Week 3 against the Green Bay Packers.[17] He finished his rookie season with 56 tackles, five sacks, a forced fumble and fumble recovery, and was named to the 2018 PFWA All-Rookie Team as a result.[18]
In Week 14 of the 2020 season against the San Francisco 49ers, Payne forced a fumble on quarterback Nick Mullens, which was recovered and returned for a touchdown by Chase Young and would also recover a forced fumble by Young.[19] In Week 15 against the Seattle Seahawks, Payne recorded his first career interception off a pass thrown by Russell Wilson during the 20–15 loss.[20] Payne finished the 2020 NFL season playing 880 snaps and recording 54 tackles, 3 sacks, 3 forced fumbles, and an interception. He also recorded two sacks against Tom Brady and the Tampa Bay Buccaneers in the wild-card round of the playoffs.[21]
The team exercised the fifth-year option on Payne's contract on April 27, 2021,[22] which guarantees a salary of $8.529 million for the 2022 season.[23] He was added to the COVID-19 reserve list on August 1, 2021,[24] before being re-activated on August 5.[25] Payne and defensive end James Smith-Williams sealed the Week 11 win over the Carolina Panthers after they sacked quarterback Cam Newton on fourth down with less than a minute and a half left in the game.[26]
By Week 9 of the 2022 season, Payne accumulated a new career-high of 5.5 sacks.[27] With 58 seconds remaining in the Week 12 game against the Atlanta Falcons, he deflected a touchdown pass attempt from Marcus Mariota which cornerback Kendall Fuller intercepted in the end zone in a 19–13 win.[28] He finished the season having set new career highs with 64 tackles, 11.5 sacks, and five pass deflections.[29] In January 2023, Payne was named as a replacement player for Aaron Donald to the 2023 Pro Bowl, his first Pro Bowl.[30]
The Commanders placed a non-exclusive franchise tag on Payne before him signing a four-year, $90 million extension with the team on March 13, 2023.[31][32]
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