In 2011, she traveled to Japan with her 90210 costars AnnaLynne McCord and Jessica Stroup to attend the Asia Girls Explosion (AGE) in Tokyo, after filming 90210's third-season finale. Grimes was caught up in Japan due to the events of the tsunami and earthquake. According to the actress, she was at Buddha's temple at the time when the earthquakes first occurred. Consequently, she started a campaign called "Spread The Heart" with the aim of supporting Japan by victim relief after the events of the tsunami and earthquakes. Many celebrities joined the campaign which later became a big movement.
In May 2011, during her 90210 hiatus, she took a six-week internship at Teen Vogue in New York City. She stated that working as an editor for a fashion magazine has always been her dream. In the fall of 2011, she directed a music video for Megan and Liz's original song "Are You Happy Now?" to raise awareness about anti-bullying, in partnership with DoSomething.org. In 2013, Grimes starred in the film Sugar about a runaway girl living on the streets of Venice, Los Angeles.