LiSA released her first full solo album Lover"s"mile on February 22, 2012; the album peaked at No. 7 on the Oricon weekly charts. She attendedShe attended the Anime Expo 2012 in Los Angeles as a guest of honor and performed her first concert in North America there on July 1. After her success with "Oath Sign", she was chosen to perform the first opening theme to the 2012 anime series Sword Art Online; the single "Crossing Field", her second single, was released on August 8, 2012; the single peaked at No. 5 on Oricon Her third single "Best Day, Best Way", which peaked at No. 6 on Oricon, was released on April 3, 2013, and her fourth single "Träumerei", which peaked at No. 15 on Oricon
On January 3, 2014, LiSA held a sold-out solo concert at the Nippon Budokan. Her fifth single "Rising Hope", which is used as the opening theme to the 2014 anime series The Irregular at Magic High School, was released on May 7, 2014; the single peaked at No. 4 on Oricon. In late 2015, she performed "ID", which is used as theme song of the 2015 video game Dengeki Bunko: Fighting Climax Ignition.
To commemorate her fifth year as a solo artist, LiSA released her Letters To U EP as a limited edition LP on March 23, 2016. LiSA released a mini-album titled Lucky Hi Five! on April 20, 2016. She released the single "Brave Freak Out", which is used as the first opening theme to the 2016 anime television series Qualidea Code, and the single also includes the song "AxxxiS", which is used as the second opening theme to Qualidea Code, on August 24, 2016. She released the single "Catch the Moment" on February 15, 2017; the title track is used as the theme song to the 2017 anime film Sword Art Online The Movie: Ordinal Scale.