Pompey manager Paul Hart has been "relieved of his duties" by the club this evening.
In a statement, the club's board said it had made the decision "reluctantly" and had based it on the team's results and league position.
Pompey are currently bottom of the Premier League with just seven points from 13 games.
Hart was offered the role of technical director, developing players from the ages of 18-21, but he declined the position.
The club said it plans to announce a replacement "very quickly".
For the moment, first team coaches Paul Groves and Ian Woan will take charge.
Chief executive Peter Storrie said: “Paul has worked under very difficult circumstances with the financial restrictions the club has faced since he took over.
“However, the board feels that the team should have accrued more points to date and that we need a new man in charge to ensure Premier League survival.
“The board would like to thank Paul for his work not only in keeping the club in the Premier League last season but also for his time in charge of youth development.
“Paul is a man of great dignity and we hoped he would stay and help us develop younger players on the fringes of the first team. We are genuinely sad to see him leave. Everyone at the club wishes him well for the future.”
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