Smart rose to prominence in 2011 after leading Virginia Commonwealth University to its first and only Final Four appearance in school history in the 2011 NCAA tournament.

This led Smart to lead a student group which held multicultural events and seminars on homophobia and racism.

He was a three-year starter as a point guard for the Panthers and set school records for assists in a game (20), season (291), and career (458).

He graduated magna cum laude with a degree in history, focusing on issues of race and the Great Migration.

Smart was a four-year starter for the Kenyon Lords basketball team, and set school records for assists in a season (184) and career (542).

[3][6] After graduating from Kenyon, Smart received an NCAA postgraduate scholarship and earned a master's degree in social science from California University of Pennsylvania.

[5] Without Sanders, the Rams went 23–11 and played in their second consecutive Colonial Athletic Association championship game, losing to Old Dominion.

In his first season at Texas, he led the Longhorns to a 20–13 record and received the sixth seed in the NCAA tournament, which the Houston Chronicle described as having "surpassed all realistic expectations.

[18] He also received commitments from Gerald Liddell, Brock Cunningham, Jaxson Hayes, and Kamaka Hepa in what was the eighth-ranked recruiting class in the country.

[21] Smart ended a three-season absence from the NCAA tournament in 2021 when he led the Longhorns to a 19–8 record and a Big 12 conference championship.

3 seed in the NCAA tournament and were defeated by Abilene Christian University in the first round, after which San Antonio Express-News reporter Nick Moyle questioned Smart's job security.

[24] Marquette University hired Smart to replace Steve Wojciechowski as the Golden Eagles' head coach in March 2021.

Smart led the Golden Eagles to 19–13 record the following season, where they lost in the first round of the NCAA tournament to the University of North Carolina.