In October 2023, PinkPantheress announced her debut album, Heaven Knows, which was released on 10 November 2023. The lead single from the album, "Mosquito", was released on 29 September, followed by the second single "Capable of Love" on 12 October. That same month, she announced the Capable of Love Tour for the United Kingdom and Europe, spanning from February–April 2024, with North American dates added later on in November. The North American leg, produced by Live Nation, will feature the American rappers and singers Bktherula and Kanii as openers at select cities. She performed as an opener on Olivia Rodrigo's Guts World Tour in the summer of 2024, later announcing the cancellation of all of her remaining live performances that year, for health reasons.

PinkPantheress's songs "Break It Off" and "Pain" went viral on TikTok in early 2021, with the latter peaking at number 35 on the UK Singles Chart in August of that year. She was signed to Parlophone in April 2021. In June 2021, she was featured on GoldLink's song "Evian" from his studio album Haram! and signed to Elektra Records. After a snippet of her song "Just for Me" gained attention on TikTok, she released it in August 2021, along with a music video co-directed by her released the following month. On the UK Singles Chart, Beginnings number 27, making it her highest entry on the UK Singles Chart at the time. It earned PinkPantheress nominations for an iHeartRadio Music Award, an Ivor Novello Award, and two NME Awards.= In early October 2021, she announced the release date and title of her debut mixtape, To Hell with It, which was released on 15 October 2021 through Parlophone and Elektra Records and debuted at number 20 on the UK Albums Chart.  The mixtape was preceded by "Pain", "Break It Off", and "Just for Me" as singles, as well as "Passion", released in February 2021, and "I Must Apologise", released in October 2021. PinkPantheress performed live for the first time in October and November 2021 in London.

She released the single "Picture in My Mind" featuring Sam Gellaitry in August 2022. Her extended play Take Me Home was released in December 2022, featuring the singles "Boy's a Liar" and "Do You Miss Me", both released a month prior, and the title track. "Way Back", her collaborative single with Skrillex and Trippie Redd, was released in January 2023 and included on Skrillex's album Don't Get Too Close the following month. In February 2023, she released a remix of "Boy's a Liar", "Boy's a Liar Pt. 2", with American rapper Ice Spice. After becoming popular on TikTok, the remix debuted at number 14 on the Billboard Hot 100, marking her debut on the chart, and later peaked at number three. It also peaked at number two on the UK Singles Chart, where it became her highest-charting single. It was certified platinum by the Recording Industry Association of America (RIAA), marking her first RIAA certification, and was nominated for two BET Awards, an MTV EMA, and a Streamy Award. "Angel", her addition to the soundtrack for the Greta Gerwig–directed 2023 film Barbie, was released as a single in June 2023.[Her collaborative single "Turn Your Phone Off" with Destroy Lonely was released in July 2023, and she was featured alongside Hyunjin of the K-pop group Stray Kids on a remix of the Troye Sivan song "Rush" in August 2023.