At the Hong Kong Tennis Classic, she joined Russia's group and won in the final against Europe with Maria Kirilenko and Yevgeny Kafelnikov. As the second seed at the 2011 Medibank International Sydney, Zvonareva received a bye into the second round, where she was defeated by Flavia Pennetta, 7–5, 7–5. Zvonareva was seeded second at the 2011 Australian Open in singles. She defeated Sybille Bammer, 6–2, 6–1, in the first round, breaking Bammer four times in a row. Zvonareva defeated unseeded Bojana Jovanovski in the second round, 2–6, 6–3, 6–1. In the third round, Zvonareva defeated 31st seed Lucie Šafářová in straight sets, 6–3, 7–6(9). Zvonareva defeated unseeded Iveta Benešová in the round of 16, 6–4, 6–1. She then defeated 25th seed Petra Kvitová in the quarterfinal, 6–2, 6–4. In the semifinal, she was defeated by third seed and eventual champion Kim Clijsters, 6–3, 6–3.
At the 2011 PTT Pattaya Open, Zvonareva was the top seed and was seeking her third consecutive title and second title defense. She defeated Tamira Paszek, 6–4, 6–2, in the first round, qualifier Nungnadda Wannasuk, 6–1, 7–5, in the second round, and Peng Shuai, 6–4, 4–6, 6–4, in the quarterfinals. In the semifinals, Zvonareva was upset by fourth seed Daniela Hantuchová, 7–6(3), 6–4. As the second seed at the 2011 Dubai Tennis Championships, Zvonareva received a bye into the second round. There, she defeated Roberta Vinci, 6–3, 6–1. In the third round, she was upset by the 15th seed Alisa Kleybanova, 6–3, 6–2.
Zvonareva picked up her first title of 2011 in late February at the 2011 Qatar Ladies Open. She was the second seed, receiving a bye into the second round, where she defeated Dominika Cibulková, 6–1, 6–2. In the quarterfinals, she defeated Daniela Hantuchová, 7–5, 6–7(5), 7–5, in a match lasting over three hours, after trailing 5–4 in the third set. She defeated former world no. 1 Jelena Janković, 6–1, 2–6, 6–4, in the semifinals, and current world no. 1 and top seed Caroline Wozniacki, 6–4, 6–4, in the final. It was Zvonareva's first title in over a year and the third time she had defeated the reigning World No. 1.
Zvonareva was the third seed at the 2011 BNP Paribas Open and had a bye into the second round. Despite letting a 6–3, 5–1 lead escape her, she defeated Timea Bacsinszky, 6–3, 7–6(4). In the third round, in a match that lasted over three hours, she was upset by 25th seed Dominika Cibulková, 4–6, 7–6(4), 6–4, despite saving five match points. Zvonareva was the third seed at the 2011 Sony Ericsson Open with a bye into the second round, where she defeated Dinara Safina, 3–6, 6–3, 6–2. In the third round, she faced 28th seed Jarmila Groth, defeating her in straight sets, 7–6(4), 6–2. In the fourth round, she faced the 15th seed Marion Bartoli, prevailing 2–6, 6–3, 6–2. Then in the quarterfinals, Zvonareva faced ninth seed Agnieszka Radwańska, whom she defeated, 7–5, 6–3, to reach the semifinals in Key Biscayne for the second time, the last time being in 2008. Despite winning two of her four previous matches after trailing a set in the tournament, Victoria Azarenka, the eighth seed, dispatched Zvonareva in the semifinals, 6–0, 6–3. Zvonareva led the Russian Fed Cup team in their semifinal tie against Italy. She defeated both Sara Errani and Roberta Vinci in straight sets to ensure a spot for Russia in the final.
Zvonareva kicked off her clay-court season at the 2011 Porsche Tennis Grand Prix in Stuttgart, Germany. As the second seed, she received a bye into the second round, defeating Anastasia Pavlyuchenkova, 3–6, 6–4, 6–2, before losing to Samantha Stosur in the quarterfinals. She was the second seed at the 2011 Mutua Madrileña Madrid Open, where she beat Patty Schnyder and Elena Vesnina, before being upset by 16th seed and eventual champion Petra Kvitová in the third round. At the inaugural 2011 Brussels Ladies Open, after a first round bye, she defeated qualifier Galina Voskoboeva, after dropping the first set in the second round. In the quarterfinals, she blew out world no. 28 and sixth seed Alexandra Dulgheru of Romania, 6–0, 6–1, losing just one point on serve. Her run ended in the semifinals, where she was upset 6–3, 6–3 by eighth seed Peng Shuai of China. Zvonareva was seeded third at the 2011 French Open and defeated unseeded Lourdes Domínguez Lino in the first round, 6–3, 6–3. In the second round, she defeated Sabine Lisicki, 4–6, 7–5, 7–5, despite trailing 5–2 in the third set and having to save a match point. Zvonareva avenged her loss at the previous year's French Open by defeating Anastasia Rodionova in the third round, 6–2, 6–3. In the fourth round, where she was the top remaining seed, Zvonareva came up against the 15th seed Anastasia Pavlyuchenkova. The match showed sporadic form by both women, until Pavlyuchenkova prevailed, 7–6(4), 2–6, 6–2.
Beginning the grass-court season at the 2011 AEGON International as the top seed, Zvonareva defeated Heather Watson, 6–3, 6–3, and Serena Williams, 3–6, 7–6(5), 7–5, but lost to Samantha Stosur, 4–6, 7–6(4), 6–4, in the quarterfinals. Zvonareva was second seed at Wimbledon, defeating Alison Riske, 6–0, 3–6, 6–3, in the first round and Elena Vesnina, 6–1, 7–6(5), in the second round, before falling to Tsvetana Pironkova, 6–2, 6–3, in a rematch of the previous year's semifinal match. Zvonareva suffered an ankle injury during her singles match and subsequently withdrew from the doubles competition.
Zvonareva's hard-court summer began at the inaugural Baku Cup, where she was the top seed. Zvonareva defeated Nigina Abduraimova, Kristína Kučová, Anna Tatishvili, and Mariya Koryttseva to reach the final, where she defeated Ksenia Pervak, 6–1, 6–4, for her twelfth WTA title. At the Mercury Insurance Open in Carlsbad, California, she was the top seed and made it to the final, where she lost to Agnieszka Radwańska, 6–3, 6–4. By making it to the final, Zvonareva achieved a career-high winning streak of nine matches. Zvonareva then went on to play in the Rogers Cup in Toronto, Canada, where she was third seed. After receiving a bye into the second round, she defeated Nadia Petrova, 7–5, 6–4, before again falling to Agnieszka Radwańska, 6–4, 7–6(4). Despite the early loss compared to her 2010 performance, Zvonareva rose to World No. 2, matching her career-high ranking. At the 2011 Western & Southern Open in Cincinnati, she was second seed and received a bye into the second round. She defeated Ekaterina Makarova, Petra Martić, and Daniela Hantuchová en route to the semifinals, where she fell to the fourth seed and eventual champion Maria Sharapova, 2–6, 6–3, 6–3. At the US Open, Zvonareva was second seed and defeated qualifier Stéphanie Foretz Gacon, Kateryna Bondarenko, 30th seed Anabel Medina Garrigues, and the 22nd seed Sabine Lisicki to reach the quarterfinals, where she lost to ninth seed and eventual champion Samantha Stosur, 6–3, 6–3. Unable to defend her runner-up points from 2010, she fell to World No. 4.
Zvonareva began her Asian hard-court swing at the Toray Pan Pacific Open in Tokyo, where she was the fourth seed and received a bye into the second round, then defeating Tsvetana Pironkova, Iveta Benešová, Maria Kirilenko, and Petra Kvitová—all in straight sets to progress to the final for the first time, where she lost to ninth seed Agnieszka Radwańska, 6–3, 6–2. She next played at the China Open in Beijing, where she was third seed and received a bye into the second round as a result of making the final in Tokyo. She lost in the third round to Ana Ivanovic. After Beijing, Zvonareva became the sixth qualifier for the year-end WTA Tour Championships. At her home tournament, the Kremlin Cup, she reached the quarterfinals, where she lost to the No. 8 seed and eventual champion Dominika Cibulková, 4–6, 6–4, 6–4.
At the WTA Tour Championships, Zvonareva was placed in the Red Group alongside World No. 1 Caroline Wozniacki, 2011 Wimbledon champion Petra Kvitová, and Agnieszka Radwańska. In Round Robin play, she fell to Kvitová 6–2, 6–4 before rebounding to defeat Wozniacki 6–2, 4–6, 6–3, her fourth victory over a reigning World No. 1. She then faced Radwańska in her final round robin match, eventually falling 1–6, 6–2, 7–5 after not able to capitalize on three match points serving at 5–3. By virtue of the highest games won percentage of her group after Kvitová, Zvonareva became the second qualifier for the semifinals from the Red Group. She lost to Victoria Azarenka 6–2, 6–3, and ended the year as World No. 7.
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