Coples was selected 16th overall in the first round of the 2012 NFL Draft by the New York Jets. He signed a four-year contract worth $8.8 million on May 17, 2012. During his rookie season of 2012, Coples compiled with 30 tackles and 5.5 sacks. The Jets finished 6–10 (tied 3rd in AFC East) that season.
With the acquiring of Sheldon Richardson in the 2013 NFL Draft, the Jets announced that Coples would transition to outside linebacker. During a preseason game against the Jacksonville Jaguars on August 17, 2013, Coples suffered a hairline ankle fracture after defending a pass thrown by Chad Henne. The Jets projected that Coples was going to be out indefinitely due to the injury but he eventually returned during Week 3 against the Buffalo Bills on September 22, 2013. During the 2013 season, Coples performed somewhat well at his new position as an outside linebacker playing 14 games (13 started) with 38 tackles, a forced fumble, 3 passes defended, and 4.5 sacks. The Jets finished 8–8 (tied 2nd in AFC East) that season.
In 2014, Coples played all 16 games with 15 starts mostly at the outside linebacker position and made 35 tackles with 6.5 sacks along with a forced fumble. The Jets plummeted to a 4-12 record, their worst record since 2007.
The Jets picked up the fifth-year, $7.8 million option of Coples' contract on April 23, 2015. Coples began to see limited playing time in 2015 due to a lack of performance as he only made 8 tackes along with a fumble recovery in 10 games. The Jets waived Coples on November 23, 2015.