The 32-year old Londoner was told that his contract at the Reebok Stadium would not be renewed last month, and is now on his way to the South West where he will link up with Bobby Williamson's team for pre-season training in just under three weeks from now.
Barness made over 100 appearances in his five years at Bolton and proved to be a reliable member of the first team squad. Williamson was delighted that both he and former Manchester United player Bojan Djordic had agreed to move to Home Park.
"Anthony has played in the Championship but the majority of his career has been in the Premiership - his experience will play a big part throughout the season.
"He can play right or left-back, which is an added bonus. I'm delighted both Anthony and Bojan have chosen to join Plymouth, they will add more quality to the squad."
Meanwhile former Wanderers reserve player Ricky Shakes has completed a much expected move to Swindon Town.