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It comes five years after quitting tennis as Barty joins Australian legends Margaret Court (1962, 1964, 1969, 1970, 1973), Evonne Goolagong Cawley (1971) and Lesley Bowrey (1963, 1965) on the Roland Garros honour roll.
Barty's victory caps off an incredible turnaround since returning to tennis in 2016 - with a ranking of 623 - after an 18-month break where she played cricket.
The new queen of clay will also pocket A$3.74 million (€2.3 million) after taking out her maiden grand slam at a tournament where the Australian had remarkably never passed the second round in five previous visits.
"This is just the start," Barty said in her victory speech.
“It’s unbelievable. I played the perfect match today ... I am incredibly proud of what I have been able to achieve in this amazing two weeks."
Barty's maiden grand slam victory rockets the 23-year-old to number two in the world and she becomes one of the early favourites to land the Wimbledon title.
Her new ranking is highest by an Australian woman since Goolagong Cawley reached top spot in 1976.
Barty also follows her idol's footsteps by becoming just the second Indigenous Australian to lift the Suzanne Lenglen Cup, after Goolagong Cawley won the title in 1971.
The Queenslander is also the first Australian singles champion in Paris since Court clinched the last of her five titles in 1973.
Barty has become only the 17th Australian woman to win a grand slam - and first since Samantha Stosur at the US Open triumph in 2011.
Samantha Stosur, Lleyton Hewitt (2001 US Open and 2002 Wimbledon) and now Barty are the only Aussies to win a major since the turn of the century.
The Ipswich-born talent powered through the first set in just under half an hour, breaking her 19-year-old opponent three times.
It was the first time Vondrousova, who was looking to become the first teenage winner since Iva Majoli 22 years ago, had dropped a set in the tournament and the loss of the second set sealed the title for Barty after 1 hour and 10 minutes.
ADDITIONAL REPORTING: AAP