James, a redshirt sophomore who is one of the top draft prospects in the country, announced his intentions in an Instagram post Tuesday.
ESPN's Mel Kiper Jr. lists James as the No. 3 overall prospect on his latest Big Board.
James was the only FSU player to earn a first-team All-ACC selection. He had 84 tackles, which was second on Florida State, two interceptions -- including one returned for a touchdown -- and one sack after missing most of 2016 with a knee injury.
James said he will not participate when Florida State plays Southern Miss in the Walk-Ons Independence Bowl on Dec. 27. He is following the same lead as Christian McCaffrey and Leonard Fournette, who both skipped bowl games last year in preparation for the NFL draft.
The Associated Press contributed to this report.