The oldest of seven children, Smith helped his single mother, who attended Rappahannock Community College in the day and worked at night, with household chores and earned honor roll grades in school.

[1] The Virginia staff, which questioned whether he had recovered his speed after a basketball injury during his junior year, asked Smith to run a 4.5-second 40-yard dash at a Nike combine at Clemson University, which he did.

[3] In summer camp, Smith adjusted from playing quarterback to wide receiver, a position he had limited experience with in high school.

[11] In its midseason report, The Baltimore Sun credited Smith for often giving an inconsistent Maryland team good field position with his long kick returns.

[19] In the latter part of the season, Smith increased his role and was elevated over Isaiah Williams as the number-two receiver across from Darrius Heyward-Bey.

Head coach Ralph Friedgen explained that his presence would alleviate the coverage on Heyward-Bey and praised Smith's blocking ability in the running game.

[20] Against Florida State, Smith broke the school record for single-season kickoff return yards, previously held by cornerback Josh Wilson.

[11] Before the 2009 season, Smith reportedly struggled in Maryland's summer camp, dividing his time between practice and online courses at night.

[25] Towards the end of camp, head coach Ralph Friedgen noted an improvement in his performance, which reestablished Smith as the team's top receiver alongside Adrian Cannon.

[37] During the game, Virginia chose to kick short to keep the ball away from Smith on kickoffs, and quarterback Chris Turner did not target him until the fourth quarter.

[41][42][43] After the season, the Atlantic Coast Sports Media Association named Smith to the All-ACC second team as both a wide receiver and return specialist.

[28] Smith returned to Maryland for the 2010 season to increase his NFL draft stock, complete his criminology and criminal justice degree in December, and improve the team's record from a 2–10 finish the year prior.

"[28] Prior to the start of the season, the coaching staff planned to increase Smith's efficiency by playing him fewer snaps in an attempt to keep him fresh.

"[52] Redshirt freshman Danny O'Brien secured the starting quarterback position after Jamarr Robinson suffered a shoulder injury, and the rookie soon "found great chemistry" with Smith.

[69] Quarterback Danny O'Brien expressed his readiness to throw deep passes to Smith in single coverage, "If it's even, I put it up.

Smith recorded a phone message and video appealing to fans in a bid to improve home attendance, which had been lackluster throughout the season.

[74] During the game, Smith set the school record for career all-purpose yardage, which surpassed Lamont Jordan's previous mark of 4,960 yards.

[73] His four touchdown receptions in a single game also set a school record, which surpassed the previous mark of three shared by Vernon Davis, Guilian Gary, Jermaine Lewis, and James Milling.

[75] Smith's season tally of twelve touchdowns also set a school record, which surpassed the mark of nine shared by Jermaine Lewis and Marcus Badgett.

[75] Upon the conclusion of the regular season, the Atlantic Coast Sports Media Association named Smith to the All-ACC first team as a wide receiver.

[88] On November 20, 2011, Smith made six receptions for a Ravens rookie record 165 yards against the Cincinnati Bengals, including a 49-yard touchdown from Joe Flacco.

[91] The morning before Baltimore's Week 3 NBC Sunday Night Football rematch with the New England Patriots, Smith's younger brother Tevin Jones died in a motorcycle accident, leaving the former distraught.

[109] In Week 13, on the first possession, Smith scored the game's opening touchdown against the San Diego Chargers, after juggling the ball in the endzone.

[110] In their regular season finale, the Ravens took on their division rivals, the Cleveland Browns, needing a win and a Chargers loss to get into the playoffs.

Trailing 10–6 in the final quarter, Smith caught a deep pass from Flacco, and on the very next play, a 16-yard touchdown to give Baltimore the lead.

[122] The following game, Smith caught six passes for a season-high 120 receiving yards and a 75-yard touchdown, followed up with a two-point conversion catch during the 49ers 43–18 loss to the Pittsburgh Steelers.

[125] On December 11, in Week 14, Smith suffered a concussion after hitting his head hard on the turf with his helmet on during a 23–17 loss to the New York Jets.

[129] On March 9, 2017, Smith signed a three-year, $15 million contract with the Philadelphia Eagles with second and third-year options at the same salary.

Smith has established a college scholarship fund to assist low-income youth from Maryland, Pennsylvania and Virginia in honor of his late brother.

Smith told Ravens coach John Harbaugh that he wanted to play in that night's game against the New England Patriots.