Former Tottenham Hotspur manager Jol, who took charge at Amsterdam Arena last year, decided to leave because he felt he wouldn't live up to Ajax's expectations.
"With pain in my heart I say goodbye to this wonderful club," he told Ajax's official site.
"We started something last summer that I would have finished. But I have come to realize that the expectations after last season were too high.
"We cannot meet such expectations. The amount of criticism that the club has had to endure daily has led to unrest in the club and among players.
"I take this decision consciously before AC Milan v Ajax (in the Champions League) is played (on Wednesday).
"The coming weeks are very important and I sincerely hope that something happens in the squad to make it in the short term a winning team."
Ajax finished their league campaign as runners-up last season, one point behind champions FC Twente.
However, Ajax's form has been fluctuating this season, which prevented them from maintaining consistency on all fronts.
They now lie fourth in the Eredivisie table with 32 points, five behind leaders PSV.