VCU sports information director Scott Day confirmed to reporters gathered at the campus Thursday night that Smart was making the move. Smart met with VCU players earlier in the evening at the Siegel Center, the team's home arena, and at least one player was seen crying when he left.
Texas athletic director Steve Patterson flew to Richmond, Virginia, on Thursday, and the Longhorns formally announced the hire on Friday.
Smart, who won at least 26 games in each of his six seasons at VCU, has been one of the hottest names in college coaching since leading the Rams to the Final Four in 2011. Patterson zeroed in on bringing Smart to Texas immediately after firing former Longhorns coach Rick Barnes over the weekend. Barnes later was hired at Tennessee.
Terms of Smart's contract were not immediately released. Barnes made $2.62 million last season. Smart made $1.8 million with the Rams.
The Longhorns will introduce Smart at a news conference on Friday.
The coach slipped into VCU's arena Thursday without speaking to the media gathered. VCU players were escorted from the meeting by university public relations and did not comment.
At VCU, Smart took over a program that had great success under Jeff Capel and then Anthony Grant. Smart hopes to avoid the pitfalls at Texas that his predecessors encountered when they left to take over programs at universities considered football schools.
Capel lasted five years at Oklahoma before being fired, and Grant spent six at Alabama before he was dismissed.
By leaving before May 1, Smart owes VCU a $500,000 buyout. His contract also contains a provision that if he became a head coach at another institution, that school would have to play VCU in a home-and-home series or pay VCU $250,000.
Smart is bolting for a Texas program that hasn't been able to unseat Kansas atop the Big 12. But the Longhorns also boast the wealthiest athletic department in the country and easy access to some of the nation's most fertile recruiting grounds in Dallas and Houston.
Barnes led Texas to 16 NCAA tournaments in 17 seasons, but his teams hadn't made it out of the first weekend since 2008.
Barnes' best years came from 2003 to '08, when Texas made its first Final Four in more than 50 years and twice more reached the Elite Eight. Texas also earned the program's first No. 1 ranking in the 2009-10 season.
But the program had plateaued, and the early-round exits in the tournament started to mount, despite rosters full of future NBA talent.
Kevin Durant, one of those NBA talents to come out of Texas during Barnes' tenure, welcomed Smart to the fold Friday.
Welcome to the family Coach Smart.— Kevin Durant (@KDTrey5) April 3, 2015
Smart is sure to energize the Longhorns.
Under him, the Rams won the CBI postseason tournament in his first season. But he really became a hot coaching commodity when VCU made its monumental run in the NCAA tournament the following season. The Rams went from being a questionable selection, barely getting a bid and playing in the First Four in Dayton, Ohio, to beating five major-conference schools to reach the Final Four.
While Barnes' stumbles in the NCAA tournament over the years played a role in his dismissal, VCU and Smart continued to pick up tournament wins. In the past five seasons, VCU went 7-5 in the Big Dance while Texas was 2-4. As a lower seed, VCU went 5-3 as Texas was 0-3 since 2011.
Beyond the Final Four run, this season might have been Smart's best coaching job at VCU.
The Rams lost Briante Weber, the leader of their "havoc" defensive style, on Jan. 31 to a knee injury and played the last month and a half with scoring leader Treveon Graham bothered by a high left ankle sprain, sometimes even sidelined.
VCU (26-10) lost six of 10 late in the season, enduring its first three-game slide in Smart's six seasons, before winning five straight, including four in four days, to win the Atlantic 10 tournament.
Smart led VCU to at least 26 wins in six consecutive seasons, a feat matched only by Duke. With the interest he has generated in basketball, a $25 million basketball practice facility is under construction and is scheduled to be ready for use in the fall.
ESPN's Jeff Goodman, ESPN Stats & Information and The Associated Press contributed to this report.