Bryant, a junior from Lufkin, Texas, was declared ineligible by the Big 12 Conference school on Oct. 7 for allegedly failing to fully disclose to NCAA investigators his contact with former NFL great Deion Sanders.
His appeal to the NCAA was denied Thursday, effectively ending his college career.
"I feel this is the best decision for me," Bryant said about his decision late Thursday. "It's what God wants me to do. I'm going to start my training Tuesday in Tampa."
Bryant was the only one of three finalists for the Biletnikoff Award, symbolic of the nation's top receiver, who returned to school in 2009.
He ends his college career with 147 receptions for 2,425 yards with 29 touchdowns.