The 60-year-old, who made his announcement three days after Albania beat Israel 3-0 away in a World Cup qualifier, said he believed he had taken the team as far as they could go.
"This is a page of my professional experience in Albania that I would never have wanted to write," he told reporters.
"I have decided to stop now because I want the best for the growth of the team...
"It is difficult for me to leave but I am conscious my cycle with this group has ended and I would like to give the chance to whoever will replace me to know the boys in the next four matches," De Biasi added.
Affectionately referred to as Gani, an Albanian form of his Italian name Gianni, one of De Biasi's first moves was to scour the Albanian diaspora to make sure the country no longer missed out on talents such as Granit Xhaka and Xherdan Shaqiri, who both play for Switzerland.
"I would like to point out I leave today without having a team to work with," he said. "I hope people will understand my decision although not everyone will accept it."
Albania were knocked out in the group stage at Euro 2016 last year after losing to France and Switzerland, although they won one game against Romania.
Arguably their most impressive win was in the qualifiers when they beat Portugal 1-0 away.
Albania are third in their World Cup qualifying group but are seven points behind second place Italy and have little realistic chance of going to Russia next year.
(Reporting By Benet Koleka; additional reporting by Brian Homewood, Editing by Toby Davis)
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