Carole & Tuesday is full of songs of various genres sung by professional singers. (Spoilers are unmarked.)
- "The Loneliest Girl", the first song that Carole and Tuesday sing together, is often considered to be one of the show's most iconic songs. With only a piano, an acoustic guitar, and the pitch-perfect vocals of Nai Br.XX and Celeina Ann, Loneliest Girl captures everything that the duo (and to an extent, the anime as a whole) is about: making pure, unfiltered music with a human voice and an instrument, no technology required.
- "Round & Laundry" is unique in that it opens with a genuine, realistic jam session between Carole and Tuesday. We hear them slowly piece the music together with a simple beat and some vocalization, before it finally culminates in a full song.
- Angela's first solo, "Move Mountains". Both the acapella version and the full version are powerful solo pieces showcasing Angela's incredible vocal range and stage presence.
- Bulldog Anthem, OG Bulldog's song that combines hip hop... and opera. It's a hilariously bizarre combination, but that's what makes it one hell of an iconic number.
- Pyotr has the high energy pop number, "Dance Tonight". The guy proves that he isn't just a social media icon, he's a genuinely talented singer and dancer. His second solo, "Love Yourself", has the all-important message of being true to yourself, something that Pyotr actively advocates.
- Despite being unabashedly obscene, "Galactic Mermaid" is a catchy, toe-tapping acapella number that never fails to get a laugh.
- "Not Afraid", the second season's ED sung by Alisa, is a surprisingly melancholic song about moving forward and overcoming trauma. While the tone and visuals are a noticeable departure from just about every other song in the show, it does a marvelous job of foreshadowing Angela's breakdown.
- "Mother", the song that ends the story, is by far the grandest, most triumphant number in the whole series. Carole and Tuesday team up with Angela, Crystal, Pyotr, GGK, Lonesome Clarence, Flora, and Desmond to sing a beautiful Pep-Talk Song about stepping up and letting your voice be heard. Throughout the series, we've only heard each of these singers individually, so to finally hear them sing together, in perfect harmony, just makes you want to stand up and applaud. It's a truly emotional finale that gloriously caps off the series on a high note.
- The second OP, "Polly Jean", is very calming and sweet, with angelic vocals provided by Celeina Ann and Nai Br.XX.