[16] The Cardinals had no immediate need for a starting-caliber defensive end, but chose to make a value pick and draft Campbell after he unexpectedly fell out of the first round and was considered the top player available at the time of their selection.
[18][19] Campbell entered training camp slated as a backup defensive end and competed against Bryan Robinson and fellow rookie Kenny Iwebema for a spot in the rotation.
[20] Head coach Ken Whisenhunt officially named Campbell a backup defensive end to start the regular season, behind veterans Darnell Dockett and Antonio Smith.
[26] On January 3, 2009, Campbell appeared in his first NFL playoff game and made two combined tackles during a 30–24 victory against the Atlanta Falcons in the National Football Conference (NFC) Wild Card Round.
[28][29] On February 1, 2009, Campbell appeared in Super Bowl XLIII and recorded two combined tackles as the Cardinals lost 27–23 in a closely contested match that was decided as time expired.
[32] Campbell entered training camp slated as a starting defensive end after Antonio Smith departed for the Houston Texans during free agency.
Head coach Ken Whisenhunt named Campbell the starting left defensive end, opposite Darnell Dockett and alongside nose tackle Bryan Robinson, to begin the regular season.
[39] On January 16, 2010, Campbell started his first career playoff game and made three solo tackles in a 45–14 loss at the New Orleans Saints in the NFC Divisional Round.
[40] Head coach Ken Whisenhunt chose to retain Campbell and Darnell Dockett as the starting defensive ends to begin the regular season, along with nose tackle Bryan Robinson.
[42] On November 29, 2010, Campbell recorded a season-high 11 combined tackles (nine solo) and sacked quarterback Jimmy Clausen during a 19–12 loss at the Panthers in Week 15.
[45] On January 6, 2011, head coach Ken Whisenhunt announced the firing of defensive coordinator Billy Davis after the Cardinals finished with a 5–11 record and allowed the third most points in the league in 2010.
[52] He finished the season with a career-high 72 combined tackles (53 solo), ten pass deflections, eight sacks, two forced fumbles, and an interception in 16 games and 16 starts.
[18][58] Head coach Ken Whisenhunt retained Campbell, Darnell Dockett, and nose tackle Dan Williams as the starting defensive linemen to begin the regular season.
[59] On September 16, 2012, Campbell collected a season-high ten combined tackles (seven solo) and recorded two sacks on quarterback Tom Brady in a 20–18 win at the Patriots in Week 2.
[63] On January 8, 2013, the Cardinals fired general manager Rod Graves and head coach Ken Whisenhunt after the team finished last in their division with a 5–11 record in 2012.
[65] Head coach Bruce Arians officially named Campbell and Darnell Dockett the starting defensive ends to begin the 2013 season.
On December 22, 2013, Campbell recorded four combined tackles and sacked quarterback Russell Wilson twice to tie his season-high during a 17–10 win at the Seattle Seahawks in Week 16.
[73] In Week 5, Campbell recorded two solo tackles, deflected a pass, and made the second interception of his career in the Cardinals' 41–20 loss at the Denver Broncos.
[76] On November 23, 2014, Campbell made six combined tackles and had a career-high three sacks on quarterback Russell Wilson during the Cardinals' 19–3 loss at the Seahawks in Week 12.
[78] Campbell finished the season with 58 combined tackles (48 solo), seven sacks, three passes defended, an interception, and a forced fumble in 14 games and 14 starts.
Bettcher chose to retain Campbell and Frostee Rucker as the starting defensive ends with Josh Mauro and Rodney Gunter sharing the role at nose tackle.
Campbell gave his approval when the Cardinals asked him to primarily play inside and had his position changed to reflect the move to defensive tackle on the team's depth chart.
[100][101] Head coach Doug Marrone chose to move Campbell back to defensive end and named him the starter to begin the regular season, opposite Yannick Ngakoue.
[102] Campbell started in the Jaguars' season-opener, against the Texans, and recorded six combined tackles and made a career-high four sacks on quarterback Tom Savage in a 29–7 road victory.
During the fourth quarter, Cardinals' quarterback Blaine Gabbert was stripped by Yannick Ngakoue and Campbell was able to recover the ball and returned it 10 yards for a touchdown.
[120][121] In the regular season finale against the Indianapolis Colts, Campbell recovered a fumble lost by Jacoby Brissett and returned it for an 8-yard touchdown during the 38–20 victory.
[131] In Week 5 against the Colts, Campbell blocked Rodrigo Blankenship's field goal and recovered late in the fourth quarter, helping the Ravens continue their rally as they were down by eight points at the time.
He finished with 49 total tackles, 1.5 sacks, one pass defensed, and 12 quarterback hits[133] On April 9, Campbell re-signed with the Ravens on a two-year deal worth $12.5 million.
Jared Campbell, a touring stand-up comedian, also played football with Calais at both University of Miami and Arizona Cardinals as a defensive back.
On January 21, 2015, it was announced that Calais Campbell had given $1.6 million to the Hurricanes to establish an endowed scholarship for defensive linemen in perpetuity at the University of Miami.