The junior from Virginia Beach, Virginia made the announcement on his Twitter account.
In the tweet posted Wednesday, Harold addresses Virginia fans and his family, friends and teammates and says, ''it's been a great ride. I have decided to enter the NFL Draft.''
The school says Cavaliers head coach Mike London is on a recruiting trip and not immediately available for comment.
Harold was one of the first top prospects London landed.
Undersized for a traditional defensive end at 6-foot-4 and 250 pounds, Harold was third on the team with seven sacks and sixth with 54 tackles overall. He had 14.5 tackles for a loss.