A source close to the Vols' program told ESPN.com's Chris Low that multiple failed drug tests led to the pair's dismissal.
"They did a lot of positive things in two years, but we have very, very high expectations for student-athletes on and off the court," Tennessee coach Bruce Pearl said before the team's end-of-season banquet, which was not attended by the two players.
Pearl said the two players did not meet his expectations after they were given every opportunity to succeed and instead will transfer to another school, though he did not specify where.
"We just felt like both University of Tennessee and the student-athletes would be better served to move on," Pearl said.
Smith spent half the season as a starting point guard, competing for time with senior Jordan Howell as he struggled with lackluster play.
The Mount Clemens, Mich., product who came in as a highly touted recruit, averaged 7.4 points and 3.2 assists last season.
Crews spent about a month on the bench with questions about whether he had a heart condition. The Hampton, Va., player was later cleared and allowed to return to play, finishing the season with an average 5.4 points and four rebounds.
Crews served a monthlong suspension before the season began for being late to several team functions and because a campus resident assistant found small amounts of marijuana in Crews' on-campus apartment. Charges were never filed against Crews, who shared the apartment with other students.
Information from The Associated Press was used in this report.