In 2008, Grimes left the series and Canada after being cast as Annie Wilson in 90210, the CW's spin-off of Beverly Hills, 90210.

She also appeared in Picture This with Ashley Tisdale and with her former Degrassi: The Next Generation co-star Lauren Collins, and then in True Confessions of a Hollywood Starlet alongside singer JoJo.

[5] She also appeared in a music video for rock band Our Lady Peace's single "All You Did Was Save My Life".

[9] 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.

[11] 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.

In 2013, Grimes starred in the film Sugar about a runaway girl living on the streets of Venice, Los Angeles.

[23] On December 20, 2019, Grimes announced on her Instagram page that she had become an American citizen, and now holds dual Canadian-American citizenship.