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The 10th-seeded Wozniacki laboured for almost three hours in a struggle which ended in front of a standing-room only crowd as she lost to her 48th-ranked opponent in their first-round match.
With her victory, the 21-year-old from Belgrade ended a poor run of form and claimed her first win since mid-January at the Australian Open.
Wozniacki had beaten the Serb in both of their previous meetings, but was burdened with six double-faults in her Rome defeat while losing serve seven times.
Russian Maria Kirilenko restored order for the seeds at the Foro Italico as the number 12 beat Spain's Anabel Medina Garrigues 6-3, 6-3. Meanwhile, German Julia Goerges advanced over Czech Andrea Hlavackova despite losing the opening set and Varvara Lepchenko of the US defeated Lesya Tsurenko 6-4, 6-2.
In the men's ATP draw, Mikhail Youzhny provided the first minor upset as he put out German 13th seed Tommy Haas 6-4, 6-3.
The 35-year-old Haas won the Munich clay title little more than a week ago and reached the third round in Madrid.
In other first-round results, Spain's Fernando Verdasco beat Argentina's Horacio Zeballos in three sets, while Frenchman Jeremy Chardy also needed three sets before beating Spaniard Feliciano Lopez 3-6, 7-5, 7-6 (7/4).
Top seed and two-time champion Novak Djokovic was due to open later in the second round against Albert Montanes while Roger Federer, seeded second, was playing Italian wild card Potito Starace.
Argentine seventh seed Juan Martin del Potro was making his return to action after a virus, taking on Russian Andrey Kuznetsov.
