Mladenovic was given little chance against the 2011 champion but claimed an excellent 7-5 3-6 6-1 triumph in just over two hours.
Li was knocked out in the quarter-finals of clay-court tournaments against Madrid and Rome in the build-up but was still expected to challenge at Roland Garros.
But after winning this year’s first major, at the Australian Open in January, the Chinese star will make an early departure from Paris, following in the footsteps of men’s champion from Melbourne, Stanislas Wawrinka, who lost to Guillermo Garcia-Lopez on Monday.
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