Adams took over the club following the departure of Harry Redknapp in October 2008; before the team’s dismal form got them one point away from the relegation zone.
“Portsmouth Football Club can confirm that Tony Adams has left his position as first team manager with immediate effect,” read a statement on Pompey’s official website.
“Director of youth operations Paul Hart will take over as caretaker manager until a new manager is appointed.”
Adams has been at Portsmouth since 2006, where he was assistant manager to Redknapp for two years.
Previously, the Arsenal legend kicked off his coaching career as manager of Wycombe Wonderers before being a trainee coach at Feyenoord and Utrecht in Holland.
A list of candidates has been mentioned for the Pompey vacancy, including former West Ham manager Alan Curbishley and ex-Chelsea boss Avram Grant.
The latter earlier worked at Portsmouth as technical director in 2006.