Robson came through three rounds of qualifying at the Australian Open, beating Melanie Oudin, Anna Floris and Olga Savchuk to advance to the main draw for the first time. She lost to thirteenth seed Jelena Janković in the first round.
Robson was selected for the first time in her career to be a member of the GB Fed Cup Team to play in the Europe/Africa Group 1 match at Eilat, Israel on 1–4 February 2012. In the group stages she played doubles with Heather Watson, defeating pairs from Portugal and The Netherlands and Israel in the group stages. Robson and Watson did not need to play the play-off match against Austria as Anne Keothavong and Elena Baltacha won their singles rubbers, and the 2–0 lead qualified the team for a place in the World Group II promotion play-off in April 2012.
Robson lost in the third round of qualfying for the 2012 French Open at Roland Garros. However she got a place in the first round of the main draw as a lucky loser when Silvia Soler-Espinosa withdrew, but then her first round match to clay-court specialist Anabel Medina Garrigues.
After a second round showing at the AEGON Classic in Birmingham (l. to Marina Erakovic), Robson came through qualifying at the 2012 AEGON International. She reached the second round before losing to Ekaterina Makarova. However, the result helped Robson break into the top 100 for the first time in her career. In the first round of Wimbledon 2012, Robson lost to Francesca Schiavone in three sets.
Immediately after Wimbledon, Robson entered the XXV Italiacom Open in Palermo where she reached her first ever WTA semi final. After beating the world number 240 Valentyna Ivakhnenko for the loss of just 1 game in the 1st round, she shocked the number 2 seed and world number 27, Roberta Vinci in straight sets to reach her first ever WTA quarter final. She continued her good form in the quarter final, where she emerged victorious against the world number 41 and number 5 seed Carla Suárez Navarro in three sets. However, her run came to an end when she lost in the semi finals to Barbora Záhlavová-Strýcová in three sets. Robson then received a wild card to enter the main draw of the 2012 Swedish Open but lost her first match against Anabel Medina Garrigues.
She received a late place into the women's singles at the London 2012 Olympics due to the withdrawal of Croatian Petra Martic. In her first round match, she beat the world number 22 Lucie Safarova in straight sets, setting up a second round encounter with Maria Sharapova. She lost to the Russian world number 3 in a tightly contested match. She also competed in the doubles competition with Heather Watson, losing in the first round to the German pairing of Angelique Kerber and Sabine Lisicki. She then received a wildcard entry into the mixed doubles with Andy Murray. They were drawn against Czech pair Lucie Hradecka and Radek Stepanek in the first round and won in three sets. In the second round the pair beat the Australian duo of Lleyton Hewitt and Sam Stosur., and reached the final by beating Germans Sabine Lisicki and Christopher Kas, where they were beaten by the Belarusian pair Victoria Azarenka and Max Mirnyi.
Robson had direct entry to the main draw of the 2012 US Open from her WTA ranking, where she defeated Samantha Crawford in the first round. In the second round she defeated former US Open Champion Kim Clijsters in Clijsters' final singles match before her retirement. Robson consequently reached the third round of a Grand Slam tournament for the first time in her career and joined Serena Williams, Lindsay Davenport, Venus Williams, Amélie Mauresmo and Justine Henin as one of the only six people to beat Clijsters at the US Open championships, and the first player to beat her there since 2003. She followed up her performance with her first victory over a top ten player, beating 9th seed Li Na in the third round in three sets. Robson became the first female British tennis player to reach this stage of a Grand Slam tournament since Samantha Smith reached the fourth round of Wimbledon 14 years previously, but she was defeated by defending champion Sam Stosur, ending her best run at a Grand Slam tournament to date.
Laura Robson's next appearance was at the 2012 Guangzhou Open where she beat the then world number 22 Zheng Jie and the number three seed Sorana Cîrstea on the way to her first WTA tour final against Hsieh Su-wei. This was the first WTA singles final for any British woman since Jo Durie in 1990. Robson was eventually defeated having saved five championship points in the second set and despite taking a 3–0 lead in the third set. The result pushed her ranking up to a career-high 57.
Laura Robson qualified for the China Open and reached the second round but she lost to Lourdes Domínguez Lino in straight sets. At the HP Open in Japan, she was seeded 8th, the first time in her career she had been seeded at a WTA Tournament. She reached the quarter-finals before losing to Chang Kai-chen in three sets, but the result ensured that she finished the year with a ranking of 53.
In October, Robson was nominated for Sports Journalists' Association "Sportswoman of the Year". In November, along with Heather Watson, won "Young Sportswoman of the Year" at the 2012 Sunday Times Sportswomen of the Year Awards. Robson was also nominated for WTA "Newcomer of the Year" and William Hill "Sportswoman of the Year" in November, winning the former award.
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