[21] In 2006, Grimes graduated from Lord Byng Secondary School and relocated from Vancouver to Montreal to attend McGill University's joint Bachelor of Arts and Science program.

[36][37] Beginning in May 2011, Grimes opened for Lykke Li on her North American Tour, and the following August her debut album was re-released through No Pain in Pop Records, in CD and vinyl format for the first time.

[42][43] Her third studio album, Visions, was released on January 31, 2012, in Canada through Arbutus Records,[44] February 21, 2012 in the United States through 4AD,[43][44] and various dates in March 2012 elsewhere.

The album's second single, "Oblivion", was named the best song of 2012 by Pitchfork[52] and was produced into a music video co-directed by Emily Kai Bock and Grimes.

[69][70] In April 2013, Grimes posted a written statement addressing her experience as a female musician as rife with sexism and expressed disappointment that her feminist stance was often interpreted as anti-male.

[91][92] The album, titled Art Angels, was released in November to favourable reviews, garnering an 88 (out of 100) rating on Metacritic[93] and the Best New Music designation from Pitchfork.

Jessica Hopper of Pitchfork described Art Angels as "evidence of Boucher's labor and an articulation of a pop vision that is incontrovertibly hers... an epic holiday buffet of tendentious feminist fuck-off, with second helpings for anonymous commenters and music industry blood-suckers".

[109] "The AC!D Reign Chronicles" were recorded over the course of two weeks during the duo's time touring Europe and were made with minimal production,[109] shot exclusively on iPhones with no crew aside from her brother, Mac Boucher, who assisted with filming.

[112] On February 2, 2017, Grimes premiered on Tidal the high budget futuristic music video of "Venus Fly", starring herself and Janelle Monáe.

Grimes stated that this first album would be "highly collaborative and [characterized by] most glorious light", with the second highlighting themes of "pure darkness and chaos".

[125][126] On June 15, 2018, she was featured in a video for Apple's Behind the Mac series on their YouTube channel, with a preview of a song from her upcoming album titled "That's What the Drugs Are For", later released as "My Name Is Dark".

[141][142] On August 13, 2019, Grimes posted an advertisement for the Adidas by Stella McCartney Fall 2019 collection on Instagram, stating that she would release the first single off her upcoming album, Miss Anthropocene, on September 13, 2019.

[178][179][180] On May 8, Grimes appeared on a Saturday Night Live sketch as Princess Peach alongside the host, Elon Musk, as Wario.

[185] She used the Discord server to tease new music frequently, and released a snippet of a song called "Shinigami Eyes" which she continued to promote in subsequent social media posts,[185] as well as an upcoming collaboration with British DJ Chris Lake.

[187] In July 2021, Grimes, alongside will.i.am, Alanis Morissette, Nick Lachey, and Rocsi Diaz were revealed as judges on Alter Ego, a new singing competition series in which the contestants make the use of motion capture technology to portray themselves as "dream avatars".

[187][190] On September 30, Grimes released a new song titled "Love" recorded in response to her separation from Elon Musk and its subsequent media attention.

[204][205][206] Grimes was an opening act on select dates for Swedish House Mafia's "Paradise Again Tour"[207] alongside Kaytranada, ZHU, and Alesso.

[203][208] The tour ran from July 29 to November 13[203][208] Grimes appeared on Bella Poarch's song, "No Man's Land" from the Dolls EP, which was released on August 12.

[212] In January 2023, Grimes gave an update on her delayed sixth album, Book 1, announcing that her career was a 'side quest' now and that her children, friends and family were her priorities.

[228] Grimes restarted songs several times, punctuated by loud yelps and screeches, telling the crowd she was experiencing speed issues with her tracks which were playing double their normal tempo and she was having trouble “doing the math”.

"[265] The Japan Times wrote that Grimes' "otherworldly, Ableton-assisted music is crammed full of hooks fit to sit alongside Rihanna and Taylor Swift in the Top 40".

[283] Before releasing her fourth studio album, Art Angels, Grimes described one of her upcoming songs as a glam rock track inspired by David Bowie and Queen.

[299] She created an alternate cover for Image Comics' The Wicked + The Divine,[300][301][302] and designed a capsule collection of t-shirts for Hedi Slimane's Saint Laurent, in 2013.

[307][308] In May 2022, she said on Twitter she was joining the board of Unicorn DAO, "to help their mission to fund/ develop female and non-binary lead [sic] art and projects".

[309] [310] Grimes's brother Mac Boucher has played a role in creating a number of her music videos including "Violence", "Go", "Realiti", and "Venus Fly", among others.

[311] She and her stepbrother, who raps under the name Jay Worthy, collaborated on the single "Christmas Song", released on the Rough Trade bonus disc of her Visions album.

[316] Grimes has been open about her past drug use, revealing intense periods during the creation of her third album Visions in 2012, during which she "blacked out the windows and did tons of amphetamine and stayed up for three weeks and didn't eat anything".

[325] In a May 2023 interview, Grimes stated that she "kinda like[s] the patriarchy", saying it was the vehicle that brought civilization although "it's sort of oppressive" and "almost all the systems of modernity [are] broken".

[326] The same year, after members of the r/grimezs subreddit documented her affiliations with far-right figures, Grimes responded, "I'm called a Nazi because I happily am proud of white culture."

Poppy's former creative director Titanic Sinclair posted a screenshot to Instagram in 2023 with a caption saying, "I think bullying your ghostwriters into NDAs and never paying them is wrong".