The world number one triumphed 6-7 (6/8), 2-6, 6-3, 6-2, 6-4 over the Greek 22-year-old who was playing in his first Slam final.
Djokovic is now just one major away from equalling the all-time record of 20, jointly held by Roger Federer and Rafael Nadal.
It was a second French Open crown for Djokovic after his 2016 victory and adds to his nine Australian Opens, five Wimbledon titles, and three at the US Open.
The 34-year-old is the first man since Rod Laver in 1969 to win all four Slams on multiple occasions and just the third in history.
He is also the first man ever to win a Slam title by twice coming back from two sets down in same the tournament.
Djokovic now has 84 career titles in total while Sunday’s win pushed him to the brink of $150 million in prize money.
“It was an electric atmosphere,” said Djokovic after the four-hour 11-minute final.
“It’s a dream. It’s difficult to win the title against a great player. It was a difficult three days physically and mentally.”
Djokovic had also spent more than four hours on court on Friday to knock out defending champion Rafael Nadal.
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