Sharapova participated in the first Grand Slam of the season at the Australian Open, where she was the 14th seed, but lost to Andrea Petkovic in the fourth round. She also had to pull out of the 2011 Dubai Tennis Championships and 2011 Qatar Ladies Open because of an ear infection. Sharapova returned to the tour in March by taking part in the 2011 BNP Paribas Open, where she was seeded 16th. She defeated former world No. 1 Dinara Safina, in the fourth round en route to the semifinal, where she lost to world No. 1 Caroline Wozniacki. At the 2011 Sony Ericsson Open in Key Biscayne, Sharapova defeated 26th seed Alexandra Dulgheru in the quarterfinals, in a match lasting 3 hours and 28 minutes. In the semifinals, Sharapova took her Australian Open reprisal on Germany's Andrea Petkovic by defeating her. In the final, she was defeated by Victoria Azarenka, despite a late comeback in the second set. With this result, Sharapova returned to the top 10 for the first time since February 2009.
During the clay-court season, Sharapova participated in 2011 Mutua Madrileña Madrid Open, where she lost to Dominika Cibulková in the third round, and the 2011 Internazionali BNL d'Italia, where she was seeded seventh. She defeated top seed Caroline Wozniacki in the semifinals and sixth seed Samantha Stosur in the final to take home the title, marking her biggest clay-court victory to date. At the 2011 French Open, Sharapova was seeded seventh. She defeated French wildcard Caroline Garcia in the second round, despite trailing 3–6, 1–4, before winning the last 11 games of the match. In the quarterfinals, she defeated 15th seed Andrea Petkovic, marking her first Grand Slam semifinal since her comeback from the career-threatening shoulder injury. She then lost to sixth seed and eventual champion Li Na, in the semifinals, ending her clay season with a win-loss record of 12–2.
At the 2011 Wimbledon Championships, Sharapova had not dropped a set entering the final, before losing to eighth seed Petra Kvitová in straight sets. This marked her first final in over three years at a Grand Slam event. Sharapova started her summer hard-court season at the 2011 Bank of the West Classic in Stanford, California. In a highly anticipated match, Sharapova lost to the eventual champion Serena Williams in the quarterfinals. In her next event at the 2011 Rogers Cup in Toronto, Ontario, Canada, Sharapova lost to Galina Voskoboeva in the third round, marking her 100th career loss.
In the 2011 first-round tie, Sharapova played Virginie Razzano of France and lost. Sharapova was supposed to play Alizé Cornet but she was suffering from a viral illness. Teammate Anastasia Pavlyuchenkova played and defeated Cornet to secure the 3–2 win for Russia against France. Sharapova continued to participate in 2012 and helped Russia to a 3–2 win against Spain in the first-round tie. Sharapova defeated Silvia Soler Espinosa in the first rubber, but was unable to play her second rubber due to illness. In 2015, Sharapova helped Russia earn a place in the semifinals after beating Pole Urszula Radwańska in the first tie and her sister Agnieszka Radwańska in the second tie. Sharapova was scheduled to play the semi-final against Germany, however, she withdrew days before the competition. She then joined the team for the final against Czech Republic and won both of her matches, against Petra Kvitová and Karolína Plíšková. Despite the 2 wins by Sharapova, Russia still lost 3–2 after losing the decisive doubles rubber.
In 2011, Sharapova was engaged to Slovenian professional basketball player Sasha Vujačić, with whom she had been in a relationship since 2009. On 31 August 2012, Sharapova confirmed that the pair had ended the engagement and separated earlier that year. Between 2012 and 2015, Sharapova dated Bulgarian tennis player Grigor Dimitrov, and, since 2018, Sharapova has been in a relationship with British businessman Alexander Gilkes.