In April 2011 Kyary participated in the charity event “One Snap for Love” to benefit victims of the 2011 Tōhoku earthquake and tsunami. In July, she released her first promo single, “Pon Pon Pon”, citing Gwen Stefani, Christina Aguilera and Katy Perry as inspirations at that time. The music video, a psychedelic tribute to kawaisa and Decora culture, was released to YouTube and became a viral hit. “PONPONPON” entered Billboard Japan’s Hot 100 chart at 72 on July 31, 2011. Her debut album, Moshi Moshi Harajuku, was released August 17, 2011, followed a week later by her autobiography, Oh! My God!! Harajuku Girl.

On December 6, 2011, her single “Tsukematsukeru” was digitally released internationally via iTunes. On December 9, Kyary Pamyu Pamyu made her American debut in Culver City, California to perform in a fashion show and play two of her songs, as well as her first time performing the single. “Tsukematsukeru” was released physically on January 11, 2012, which included a special edition photobook. It was eventually certified gold in April 2012. In February and March 2012, she represented Japan during Japanese performing arts exhibitions in Shanghai and Hong Kong. She released her second single, “Candy Candy” as a digital download on March 14, 2012. The single debuted at eighty-nine on the Billboard Japan Hot 100, and later peaked at number two. It was released as a CD single on April 4, 2012, and sold 9,913 copies its first week, debuting at number eight on the Oricon weekly singles chart.

Her debut full-length album, Pamyu Pamyu Revolution, was released on May 23, 2012. Along with the announcement of her second single back in February, it was revealed that she was planning to hold her first nationwide tour in June of that year, as well as launching an official fan club. The tour kicked off on June 2 at the Namba Hatch in Osaka. It continued in Hiroshima, Nagoya, Sendai, Sapporo, Fukuoka and finished in Tokyo on June 29. In July 2012, she made her European debut by performing for 13,000 fans at the Japan Expo in Paris. Kyary Pamyu Pamyu was bestowed the title of “Kawaii Harajuku Ambassador” on August 30, 2012 by the Mayor of Shibuya. Following a montage of her successes performed on a large screen, she performed several songs in front of a crowd after accepting the award. In early September 2012, Kyary announced that she was collaborating with Japanese budget fashion brand g.u. for her new single “Fashion Monster”, which was given a CD release date of October 17, 2012. She was also used as the image character for g.u. after the announcement. Around the same time, Kyary Pamyu Pamyu announced her debut world tour titled 100% KPP World Tour, which began in February 2013 and lasted until June. The tour visited the United States, United Kingdom, France, Belgium, Taiwan, Thailand, Singapore, Hong Kong, and her native Japan.

During 2012 and 2013, she began receiving more attention in Western media. Sputnikmusic listed Pamyu Pamyu Revolution as number one on their “Best Pop Albums of 2012” list. Britain’s Dazed & Confused magazine became an enthusiastic supporter. Kyary was photographed by Matt Irwin for the magazine’s December 2012 issue, styled by Nicola Formichetti. The magazine also cited her video for “Furisodation” in their “Video of the Week” category in January 2013, and named her “The Star of Tomorrow” in August. In January 2013, MTV Iggy called Kyary “the coolest girl on the planet” and The Fader called her “the most exciting person making music”. Furisodeshon’s video was also named by Stereogum as a “Video of the Week” in January. Elle France promoted Kyary Pamyu Pamyu in its February 2013 issue, and she appeared on the French television show Le Petit Journal on February 11. During this period, she also appeared in the Swedish newspaper Svenska Dagbladet and was interviewed on the British radio station Monocle 24. February also saw the release of Kyary’s first concert DVD/Blu-ray, Dokidoki Wakuwaku Pamyu Pamyu Revolution Land, recorded live in November 2012 at the Nippon Budokan in Tokyo. A month-long exhibition in March 2013 titled “Kyary Pamyu Pamuseum” was held in Tokyo’s Roppongi Hills complex, showcasing all costumes from her music videos and live performances. In April, a deal for American distribution was reached with Sire Records, and “Fashion Monster” was re-released in the United States. In summer 2013, Pamyu Pamyu’s television series TV John! was broadcast in France on the Nolife channel. In America, Paper featured her in its July issue, and she received her largest American exposure to date in a lengthy profile in The Wall Street Journal the same month.

Kyary performed her songs “Invader Invader” and “Ninja Re Bang Bang” at the end ceremony for the 2013 MTV Video Music Awards Japan Awards, where she also received the awards for Best Pop Video and Best Karaoke! Song for “Fashion Monster”. In late June, it was revealed that she is working on a documentary film that is due out late 2013 entitled Kyary Pamyu Pamyu the Movie. The film featured one-day limited screening and concert footage from Kyary Pamyu Pamyu’s 100% KPP World Tour. Internationally the same year, she was nominated for Best New International Pop Artist by Fuse TV and Best Japan Act at the 2013 MTV Europe Music Awards. Kyary’s second studio album, Nanda Collection, was released on June 26, 2013. In September 2013, she announced a second world tour titled Nanda Collection World Tour and a new single “Mottai Night Land” was released in late October and received positive reviews from Western media outlets. The single was released on November 6. The world tour visited the United States, Canada, Australia, England, France, Germany, Taiwan, Thailand, Singapore, Hong Kong, and Kyary’s native Japan, lasting from February until November. It was originally to last until June but was postponed due to political unrest. She was interviewed by or was the focus of articles in internationally renowned publications such as The Guardian, Time Out London, Sydney Morning Herald, and VICE. in April 2014, Kyary Pamyu Pamyu made her Australian television debut on the program Sunrise and was the focus of Australian news programs such as ABC News. In May 2014, she appeared in the British fashion magazine i-D. In July 2014, Vogue premiered Kyary’s first English-language song, “Ring A Bell,” in the United States. In October 2014, she was the focus of an article and photoshoot in the American fashion magazine Nylon.

In February 2014, Kyary announced her single “Yume no Hajima Ring Ring” in which her theme would be “evolution” which provides a theme relating to graduation. The music video was uploaded to YouTube on February 19. The single was released on February 26. In March, she announced that her upcoming single “Family Party” will be used as an ending theme for the movie Crayon Shin-chan: Serious Battle! Robot Dad Strikes Back. Kyary has stated that this is her first original theme song for a film. “Family Party” was released on April 16. On May 9, she announced her first limited-run single, “Kira Kira Killer”, which was released on June 11. The single was featured in commercials for au’s “Lucky” campaign. Also in May, Dazed & Confused announced that Kyary was working with international musicians Sophie and Yelle on new upcoming music. she announced at her Zepp Tokyo concert that she would be releasing her third full album, titled Pika Pika Fantajin on July 9, 2014. Along with the album announcement on May 18, Kyary also announced that she would be holding an arena tour after her hall tour in Japan. Both nationwide tours were held after the Nanda Collection World Tour. The Hall tour consisted of 17 shows in 13 cities, visiting Saitama, Tokyo, Miyagi, Matsudo, Hokkaido, Tochigi, Niigata, Ishikawa, Yamanashi, Chiba, Hiroshima, Kagawa, and Aichi, and lasting from July 27 until September 22. The arena tour consisted of nine shows in five cities, which ran from October 18 to November 9, visiting the cities of Makuhari, Osaka, Nagoya, Fukuoka, and Yoyogi.

In January 2015, she was mentioned by The Hollywood Reporter as one of the “major recent sellers” for Warner Music Group alongside artists including Coldplay and Ed Sheeran. In March 2015, Kyary Pamyu Pamyu released her single “Mondai Girl”. In June, she was chosen by the international cosmetic brand MAC Cosmetics as one of its “Global Heroes” and was profiled in an interview on their website. In the following month, Kyary was chosen to represent Japan in Italy at Expo 2015. On June 17, 2015, a remake of the movie Nutcracker Fantasy with a remix of her song “Oyasumi” as the theme song. On September 2, 2015, Kyary released the Halloween-themed single “Crazy Party Night (Pumpkin no Gyakushū)” and began the Crazy Party Night 2015 Tour, a nationwide concert tour that lasted until December 2015. The music video for the single premiered beforehand on August 20, 2016 and has since amassed over thirteen million views as of May 2018. On October 11, 2015, she played a one-off international concert at The Roundhouse in London, England. In November 2015, Kyary was featured prominently in advertising for “The World Goes Pop” exhibition at the Tate Modern national art gallery in London.

On May 25, 2016, her debut compilation album KPP Best was released, featuring her single “Sai & Co” which was released on April 20. Around that time, Kyary Pamyu Pamyu announced a third world tour titled the Five Years Monster World Tour. The world tour visited Singapore, London, Sydney, Melbourne, San Francisco, New York City, Taipei, and Tokyo. Her first art exhibition titled the Kyary Pamyu Pamyu Artwork Exhibition 2011–2016 was held at Laforet Harajuku from December 16. In addition to every CD jacket design being present at the event, there will be well over 100 images on display including photos from Kyary’s photobooks that are available exclusively within her album releases, outfits and wigs worn by Pamyu Pamyu herself, interactive displays of the jacket images, and much, much more. This is the ultimate Kyary Pamyu Pamyu artwork exhibition collecting together 5 years of work since her debut. In conjunction with the exhibition was released the book “Kyary Pamyu Pamyu Art Works 2011–2016”, compiling around 300 unseen images from her photobooks. It is Kyary’s first release together with art director and designer Steve Nakamura, who has been responsible for the art direction of Kyary’s releases since her debut in 2011.

On December 27, 2016, she announced that she would be collaborating with English singer Charli XCX on Yasutaka Nakata’s solo track “Crazy Crazy”. The song was released on January 18, 2017, followed later in January by her single “Harajuku Iyahoi”. In April 2017, Kyary released the single “Easta”. From August 12, 2017 to October 1, 2017, the new exhibition titled the Kyary Pamyu Pamyu Art Exhibition 2011–2016 in Taipei was released, the event will feature displays of all 18 CD sleeves since her debut back in 2011, as well as outfits and wigs worn by Kyary Pamyu Pamyu herself in music videos, unreleased works from photo books that come with her albums and more. Kyary also embarked on a tour titled The Spooky Obakeyashiki: Pumpkins Strike Back in 2017. The following year, she performed at 6 international concerts in London, Cologne, Berlin, New York, San Francisco, and Los Angeles as The Spooky Obakeyashiki World Tour. In an interview with Billboard Japan, Pamyu Pamyu stated that although her music and performance style have evolved, she hopes to “maintain that basic ‘kawaii’ side” her music and style is known for. Over a year since the release of “Easta”, she released the single “Kimino Mikata” on April 11, 2018, along with an accompanying music video.

In September 2018, Kyary Pamyu Pamyu released her fourth studio album Japamyu, her first studio album in four years. The album included her 2016 single “Sai & Kou” as well as “Harajuku Iyahoi” and “Kimino Mikata”. Kyary performed a new song from the album titled “Kizunami” on Music Station on September 7. On that same year, her contract with WMG expired.

On March 20, 2019, Kyary announced a new concert tour, “Oto no Kuni Live Tour”, which commenced on March 30 at Izumo-taisha Shrine in Shimane. On May 10, she released an independent digital single “Kimi ga Iine Kuretara” as a tie-up song to the Japanese drama Mukai no Bazuru Kazoku. In January 2020, Kyary Pamyu Pamyu was announced as a performer at Coachella 2020 in Indio, California. Due to the COVID-19 pandemic, the “Kamaitachi Tour” was cancelled and overseas shows were also postponed. Unable to perform live for everyone during the current situation, Kyary released a curated selection of her past live concerts on YouTube from April 14 to May 17, 2020.

Kyary released a digital single “Kamaitachi” on April 24, 2020 with its accompanying music video premiering on YouTube the same day. On September 12, 2020 Kyary Pamyu Pamyu launched her new fragrance brand ‘Nostalgia Syndrome’. The brand was backed by a crowdfunding campaign in February 2020 for Kyary who wanted to turn her favourite scent, fragrant olive, into a fragrance.