Smith, who left the Trotters last season and signed a short term contract at Preston North End, has put-pen-to-paper on a one year contract at Vale Park.
"Jeff is a player with Premiership qualities who has been on the fringe of the first team at Bolton," said Vale boss Dean Glover.
"He has now agreed to join us and we are delighted to have got a player like Jeff," he told the club's website.