Following men's third seed Stan Wawrinka's exit on Monday, fellow Australian Open champion Li became the biggest early victim in the women's draw as 21-year-old Mladenovic stormed through the third set.
It was another disappointing exit for Li, who won in Paris in 2011 but hasn't been past the fourth round in six other appearances.
On Tuesday, she committed 37 unforced errors. Mladenovic now meets Alison Riske of the United States in the second round. "It's just incredible, I don't have the words to describe what happened," a tearful Mladenovic said.
"To beat the world number two in the first round at Roland Garros is incredible. Without you, I couldn't have done it," the 2009 French Open junior champion told the crowd.
The 21-year-old dug deep to steal the first set from under Li's nose when she saved two set points at 5-4 before levelling the match.
It was a mighty effort from the 1.84m (6ft) right hander and she seized on a lapse by Li to close out the set 7-5 in just over an hour.
Li, who came into the tournament in good form, having reached the quarter-finals at Rome and Madrid as well as the Miami Masters final where she lost to Serena Williams, immediately hit back to start the second set.
The 32-year-old from Wuhan picked up an early break to race into a 3-0 lead which she protected the rest of the way to level the match 6-3.
Mladenovic, who teamed up with Canadian Daniel Nestor to win the Wimbledon (2013) and Australian (2014) mixed doubles titles, was the first to draw blood in the final set when she broke in the fourth game to jump into a 4-1 lead.
The match was slipping away from the Australian Open champion while Mladenovic grew in confidence knowing victory was within her grasp.
However the Chinese world number two was unable to muster a fightback as Mladenovic, who has only reached the second round twice now in six appearances at Roland Garros, closed out the match 6-1 for her most memorable singles' victory.
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