The 6-foot-6 Barry, who averaged 19.7 points per game before a season-ending shoulder injury in January, will graduate with a 4.0 GPA. He redshirted his freshman season.
Barry will be eligible to play next season as a graduate transfer student and likely will be pursued by numerous high-major schools.
"Decisions of this magnitude are never easy and today is bittersweet for me," Barry said in a statement. "I informed Coach [Earl] Grant and my teammates that I plan on graduating from the College of Charleston this summer and pursue a master's degree in nuclear engineering, mechanical engineering or physics. I am hoping to use my last season of basketball eligibility to start work on my master's program."