"Greek football mourns the loss of Alketas Panagoulias who was a pioneer," the Hellenic Football Federation said in a statement on Tuesday.
"This brings great sadness to the football family in our country."
Panagoulias led his nation to their first major championship finals, at Euro 1980.
He began his career as a left back for Aris Salonika. After his playing days ended he moved into coaching and became assistant to Greece coach Billy Bingham in 1972.
Panagoulias took over the reins a year later and guided the team to the European championship finals in Italy in 1980.
He won three league titles in two spells with Olympiakos Piraeus in the 1980s and also coached United States from 1983-85.
Panagoulias then agreed to become Greece coach for a second time and steered them to their first appearance at a World Cup finals, in the U.S. in 1994.
Following his retirement he served as president of Aris in 2002.