Ivanovic had her chances, most notably when serving more the match in the third set, but Larcher de Brito was not to be denied, triumphing 6-4, 3-6, 7-6(6) after two rollercoaster hours.
Ivanovic struggled to make an impression with her return in the second set, but was rewarded for her persistence when a couple of trademark forehands brought her the decisive break.
The former World No.1 cranked the pressure up another notch in the decider, pinning Larcher de Brito back to build an early lead. However, with the finishing line beckoning, the Serb went back into her shell, twice surrendering a break advantage.
There was time for more drama in the tie-break, Ivanovic saving two match points before finally succumbing with a double fault.
"It's an unbelievable feeling - it was so nerve-racking towards the end of the tie-break," Larcher de Brito said. "I felt a lot better in my game after qualies and beating a couple of good players.
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