A patriarch of one of Greece's most influential political families, Mitsotakis quit politics in 2004, aged 85, after serving as the country's longest-serving parliamentarian.
"He died at 0100 surrounded by the people whom he loved and who loved him," a family statement said. It did not indicate the cause of death.
The conservative politician was prime minister from 1990 to 1993 and served without interruption as an MP from 1946 on the ticket of several different parties, except for a ten-year break during and immediately after Greece's 1967-1974 military junta.
One of Greece's few openly pro-US politicians at the time, Mitsotakis cultivated close ties with the family of former president George H.W. Bush and frequently hosted them at his home in Crete.
This did not prevent him from also forging close relations with Serbian strongman Slobodan Milosevic and supporting him during the wars that tore apart Yugoslavia in the 1990s.
On the domestic front, Mitsotakis championed a tight budget and privatisations that sparked major union strikes and protests.
"You were always ahead of your time," New Democracy press chief Makarios Lazaridis said Monday.
His support for budget cuts earned him the nickname "Dracula" from his enemies. To his friends, he was often known as "the tall one" due to his imposing height.
His government eventually collapsed over a name dispute with Macedonia that continues to poison relations with the neighbouring country.
A lawyer by training, during World War II Mitsotakis was active in the resistance against the Nazi occupation on his native island of Crete.
In 1967 he was arrested by the junta but managed to escape to Paris, where he lived in exile until his return to Greece after the re-establishment of democracy in 1974.
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