She played leading roles in several anime series, including Meiko "Menma" Honma in Anohana, Inori Yuzuriha in Guilty Crown, Alice Zuberg in Sword Art Online: Alicization, Utaha Kasumigaoka in Saekano: How to Raise a Boring Girlfriend, Mashiro Shiina in The Pet Girl of Sakurasou, Saori Takebe in Girls und Panzer, Shiro in No Game No Life, Darkness in KonoSuba, Juliet Persia in Boarding School Juliet, and Mamako Oosuki in Do You Love Your Mom and Her Two-Hit Multi-Target Attacks?.
Kayano wanted to work in a job that would involve "healing people", leading to initially take up a course at a vocational school.
Kayano, Haruka Tomatsu and Saori Hayami performed the series' ending theme "Secret Base – Kimi ga Kureta Mono (10 years after Ver.
[7] She and Satomi Satō performed the series' ending themes "Madoromi no Yakusoku" (まどろみの約束) and "Kimi ni Matsuwaru Mystery" (君にまつわるミステリー).
[11] She played several roles in 2013, including Ai Fuyuumi in Oreshura,[12] and Chisaki Hiradaira in Nagi-Asu: A Lull in the Sea.
In 2016, Kayano hosted a show titled "Kayanomi ~Kayano Ai ga Nihonshu wo Nominagara, Taberu dake~~" (かやのみ 〜茅野愛衣が日本酒をのみながら、食べるだけ〜, lit.
[26] In 2021, controversy arose on Chinese social media as a result of Kayano's post regarding her February 11 trip to the Yasukuni Shrine, a Shinto shrine often a subject of controversy which enshrines Japanese men, women, children, and soldiers who died in numerous wars involving Japan spanning between the Meiji and Showa eras, including 1,068 convicted war criminals that were sentenced to death by the International Military Tribunal; of which 14 of them, including former Japanese Prime Minister Hideki Tojo, are labeled as A-Class criminals.