He garnered honorable mention all-league accolades on defense as a sophomore starting at safety, when he had 45 tackles and four interceptions on the season-his first year playing football.

Again Smith closed the season with fireworks against Nebraska, sniffing out an ill-advised fake field goal attempt by the Huskers, intercepting the lateral and taking it 58 yards for a touchdown.

During that span Smith made quite a name for himself totaling 70 tackles in both seasons defending 15 passes and posing such a threat to offenses he was thrown at a mere 20 times as a senior in man coverage.

[7] As a top cornerback prospect, Smith was one of 56 collegiate defensive backs to attend the annual NFL Scouting Combine in Indianapolis, Indiana.

[9] Smith attended private workouts and meetings with 12 teams that included the Detroit Lions, Minnesota Vikings, New York Jets, San Diego Chargers, Oakland Raiders, Washington Redskins, Cincinnati Bengals, Baltimore Ravens, Cleveland Browns, and Philadelphia Eagles.

It was reported multiple teams removed Smith entirely off their draft boards due to his history of arrests, failed drug tests, and suspected maturity issues.

Throughout training camp, Smith competed for snaps and began the regular season as the backup behind starting cornerbacks Lardarius Webb and Cary Williams.

[27] He returned the ball 16-yards before having it stripped from his grasp by Bengals' wide receiver Jerome Simpson, but it was subsequently recovered by Ravens' linebacker Brendon Ayanbadejo.

[28] On December 4, 2011, Smith earned his first career start and recorded one tackle, a pass break up, and an interception during a 24–10 victory at the Cleveland Browns.

[30] The following week, he started his first career playoff game and made a tackle, broke up a pass, and intercepted Tom Brady in the end zone after it was tipped by teammate Bernard Pollard in the fourth quarter of the Ravens' 23–20 loss to the New England Patriots in the AFC Championship.

[31] Smith entered training camp under new defensive coordinator Dean Pees, and competed against Cary Williams for the job as the starting cornerback.

On February 3, 2013, Smith recorded a solo tackle and two pass deflections during the Baltimore Ravens' 34–31 victory over the San Francisco 49ers in Super Bowl XLVII.

[36][37] In the Baltimore Ravens' season-opener at the Denver Broncos and recorded six solo tackles, a pass break up, and forced a fumble during their 49–27 loss.

Smith recorded his first interception of the season in Week 6 against Green Bay Packers quarterback Aaron Rodgers when he picked him off in the end zone.

In a season-ending loss in week 17 versus the Cincinnati Bengals, he recorded his second interception of the year when he picked off an Andy Dalton pass in the end zone.

[25] He entered training camp slated as the starting cornerback after Corey Graham departed for the Buffalo Bills in free agency.

[39] Head coach John Harbaugh named Smith the starting cornerback, opposite Lardarius Webb, entering the regular season.

On October 12, 2014, he collected five solo tackles, a pass breakup, and made his first and only interception of the season as the Ravens' routed the Tampa Bay Buccaneers 48–17.

[42] On November 6, 2014, the Baltimore Ravens announced that they would be placing Smith on injured reserve for the rest of the season after it was discovered that his foot injury would require surgery.

Bengals 28-24 Ravens (Sep 27, 2015) Final Score On October 11, 2015, Smith collected a season-high nine combined tackles in a 30-33 loss to the Cleveland Browns.

He finished the 2015 season with 54 combined tackles (48 solo), ten pass deflections, a career-high three interceptions, a sack, and a touchdown in 16 games and 16 starts.

[48] He started the Baltimore Ravens' season-opener against the Cincinnati Bengals and recorded three solo tackles, a pass deflection, and made an interception off of quarterback Andy Dalton in the fourth quarter.

[49] In Week 5, teammate Patrick Onwuasor forced a fumble and it was recovered by Smith and returned 47-yards for his second career touchdown during a 30–17 victory against the Oakland Raiders.

On October 26, 2017, Smith collected a season-high four solo tackles, broke up three passes, and returned an interception for a 50-yard touchdown as the Ravens' routed the Miami Dolphins 40–0.

Injuries, the emergence of fellow corner Marlon Humphrey, and the acquisition of Marcus Peters limited the play of Smith throughout the 2019 season.

[55] He did record an interception which he returned for 7 yards in the closing moments of the Ravens' Week 12 45–6 blowout win over the Los Angeles Rams.

He started and played every snap in the final two games of the year due to Ravens suffering numerous injuries in their secondary, including the loss of Marcus Peters and Marlon Humphrey.