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Fourth seeds Coco Gauff and Jannik Sinner, along with home hope Alex de Minaur and world number 11 Barbora Krejcikova progressed.
Coco Gauff won the final 10 games of her match against Elise Mertens, completing a 3-6, 6-3, 6-0 comeback
Having retired in 2020 to raise a family and playing in just her third event since returning to action Wozniacki turned back the clock to come out on top in the battle of 33-year-old Grand Slam champions.
Wozniacki said she would first play at the Canadian Open in Montreal in August before targeting the US Open while her long-term goal is the 2024 Olympics in Paris.
Caroline Wozniacki said that the three-set grinder against Ons Jabeur was a fitting end to her career.
The 29-year-old, who triumphed in Melbourne last year, said her retirement had nothing to do with her health and that she wanted to accomplish more in life off the court with her husband David Lee, a professional basketball player.
Diagnosed with rheumatoid arthritis at the end of last season, Wozniacki has struggled for consistency this term.
The win improved Rafael Nadal's Roland Garros record to 87-2.
Five-time Grand Slam champion Sharapova, who won her last major at the 2014 French Open, hit 37 winners against 10 from her opponent and converted her second matchpoint to set up a fourth round clash with Australian No. 1 Ashleigh Barty.
Caroline Wozniacki's honeymoon on grass was short-lived as she became the 11th women's seed to fall on the first three days at Wimbledon.