In 2010, Barretto returned to do another episode in Maalaala Mo Kaya portraying a widow who falls in love with a parish priest, which was portrayed by Jomari Yllana. Barretto again won another the award for Best Single Performance by an Actress in the PMPC Star Awards for Television, marking her second win in this category. Barretto embarked in her biggest television project in 2010 with the drama series Magkaribal, which originally featured Barretto opposite sister Claudine, however, the latter moved to rival network GMA during the show's pre-production. Magkaribal starred Barretto alongside actress Bea Alonzo (who became Claudine's replacement), Angel Aquino and model-actor Derek Ramsay. In that same year, Bench launched Barretto's first perfume line called Greta. Barretto won the award for Best Drama Actress in the PMPC Star Awards for Television for Magkaribal a year later. After the success of the show, Barretto was slated to star in Alta, a drama series about high society and the mining industry, with KC Concepcion and Angelica Panganiban, but the show was shelved in 2012. It was because of the cancellation of Alta that she was offered the role of Ashi Behati in Princess and I in which she portrayed the main villain to the lead stars Kathryn Bernardo and Daniel Padilla. In 2013, Barretto joined the cast of Huwag Ka Lang Mawawala at the request of the show's lead actress, Judy Ann Santos. Two months later, Barretto debuted in her first Cinemalaya movie entry entitled The Diplomat Hotel. She is set to portray Valentina, the nemesis of superheroine Darna in the Angel Locsin-starrer, Darna produced by Star Cinema to be released in 2015.