On 22 May 2009, de Brito qualified for her first Grand Slam tournament main draw at the French Open after winning the final round of the qualifying by beating world No. 152 Kristína Kučová, world No. 177 Yuliana Fedak and world No. 151 Ekaterina Ivanova. She became the first Portuguese female player ever to do so. After overcoming Melanie South in the first round, Larcher de Brito once again made history by becoming the first Portuguese player overall to qualify for the third round of a Grand Slam by beating world No. 15 Zheng Jie. She would lose to home player Aravane Rezaï, a game in which her opponent made a number of complaints about the amount of noise coming from the Portuguese. With her third round result, she entered the top 100 for the first time, a ranking of world No. 90.