Grimes appears in the 2010 silent fashion short film Unzipped. She wrote and directed a 2010 music video for her song "Myself and I", which features an appearance by her 90210 co-star Ryan Eggold. She also participated in YouTuberFreddie Wong's video "Gun Size Matters". She made a cameo in the horror film Scream 4, released in April 2011.
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 earthquakes. 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 & Liz's original song "Are You Happy Now?" to raise awareness about anti-bullying, in partnership with DoSomething.org.
Grimes began dating British model and musician Josh Beech in March 2012. In December 2012, after nine months of dating, Grimes announced that she and Beech were engaged. They were married on May 10, 2013 in Ashford, Kent, England.
Best Young Ensemble Performance in a TV Series (Comedy or Drama)
Degrassi: The Next Generation
(Shared with: Dalmar Abuzeid, John Bregar, Deanna Casaluce, Daniel Clark, Lauren Collins, Ryan Cooley, Marc Donato, Jake Epstein, Stacey Farber, Aubrey Graham, Jake Goldsbie, Jamie Johnston, Shane Kippel, Andrea Lewis, Mike Lobel, Miriam McDonald, Melissa McIntyre, Daniel Morrison, Adamo Ruggiero, Cassie Steele and Sarah Barrable-Tishauer)