Zidane called a news conference just an hour-and-a-half before announcing his decision, in which he said: "I have taken the decision to not continue going into the next season".
He leaves having guided the Spanish club to three successive Champions League titles and one La Liga success.
"It is the moment to make a change". After doing three years, it's the right decision.
Zidane was locked in a meeting with club president Florentino Perez on Thursday morning, sources close to the club. "I spoke with (Sergio) Ramos who respected my decision and wished me luck". We always want more from the players, and a moment comes when I can not ask them for more.
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"It is a sad day, for me, for the club, the players, everyone at this club".
Zidane led Madrid to a treble of European triumphs in Kiev last Saturday night, enshrining his side as the greatest of the modern era in Europe's elite club competition and placing them in the same bracket as the Ajax and Bayern Munich sides that achieved the same remarkable feat in the 1970s. If I don't think that we can keep winning then it's time. "They are one of the teams I loved as a kid but I felt it was a very sensitive period for Arsenal", he told beIN sports.
Zidane, 45, took over after Rafael Benitez was sacked and was in charge for 149 games.
Zidane's retirement as a Real Madrid player in 2006 also came as a surprise, when the then 33-year-old made a decision to hang up his boots in the aftermath of that year's World Cup final despite having another year on his club contract.