Manager Dean Holdsworth will have to find "another success story" after Darren Jones used Twitter to confirm he is leaving Aldershot.
The club captain, who was out of contract this summer, missed only four league games last season and was named the Players' Player of the Year and Supporters' Player of the Year.
Jones, 28, has made more than 350 career appearances and was part of the team which knocked West Ham out of the League Cup last term before they were beaten by Manchester United in the fourth round.
Jones tweeted: "Would like to thank everyone at Aldershot. Had two great seasons there. Great club, great people. All the best in the future."
Holdsworth added on the club's official website: "We made Darren a good offer and I valued him highly. A part of me is pleased for him and a part of me is disappointed to lose a player of his calibre. The fans will remember Darren fondly and we wish him all the best for the future.
"We have to turn this into a motivation to find another success story for us and that is what we will attempt to do and what I have been doing since the end of the season as it was in the back of my mind that this situation may arise."