- Composes "Quando Chegares", his first song (music and lyrics). Meetingw with Sylvia Telles, João Gilberto, Lúcio Alves, Luiz Eça, João Donato and others around the piano of Johnny Alf, at the bar in the Hotel Plaza.
- Silvinha Telles records “compact” record with "Menina" by Carlos Lyra and "Foi a Noite", by Antonio Carlos Jobim and Newton Mendonça.
- Composes "Maria Ninguém" among other songs with his own lyrics.
- Vocal group “Os Cariocas” records his song "Criticando".
- First songs written with Ronaldo Bôscoli: "Lobo bobo", "Se é tarde me perdoa", etc.
- First songs written with Geraldo Vandré: "Quem Quiser Encontrar o Amor" and "Aruanda".
- Records first LP: “Carlos Lyra Bossa Nova" with cover notes written by Ary Barroso.
- First songs with Vinícius de Moraes: "Você e eu", "Coisa Mais Linda", "Minha Namorada", etc.
- Composes music for play, "A Mais Valia vai Acabar, seu Edgar", by Oduvaldo Vianna Filho, directed by Chico de Assis.
- Composes with Maria Clara Machado the children’s musical, "Maroquinhas Fru-Fru".
- Records his second LP “Carlos Lyra”, with cover notes by Vinicius de Moraes.
- Double compact, 45 rpm, “No Balanço do Samba”, released on the Philips label, with: “Canção do olhar amado”, “Chora tua tristeza”, “Quando chegares” e “Só mesmo por amor”.
- Founds, together with Oduvaldo Vianna Filho, Ferreira Gullar and others, the Popular Center of Culture (Centro Popular de Cultura – CPC) of the National Student Union (União dos Estudantes – UNE).
- Composes music for the play “Cinderela” by Maria Clara Machado.
- Writes the musical “Um americano em Brasília together with Chico de Assis and Nélson Lins e Barros.
- Composes the music for the play “O testamento do cangaceiro” by Chico de Assis.
- Composes music for the play “Almas mortas” by Nikolai Gogol, staged by the TBC and directed by Flávio Rangel.
- Records third LP, "Depois do Carnaval".
- "Bossa Nova Mesmo" record is released with performances by Carlos Lyra, Vinicius de Moraes, Sylvia Teles, Lucio Alves, among others.
- Appears at the Bossa Nova Concert in Carnegie Hall, New York.
- Composes, together with Vinícius de Moraes, the musical "Pobre Menina Rica".
- “Carlos Lyra”, a double compact on the Philips label is released with “Você e eu”, “Chora tua tristeza”, Ïnfluência do jazz” and “Depois do carnaval”.
- Composes score for film “Gimba”, directed by Flávio Rangel.
- "Couro de Gato", with score by Carlos Lyra, receives awards at the festivals of Sestri Levanti (Italy) and Oberhausen (Germany).
- Composes with Vinícius de Moraes the "Hino da UNE" and "Marcha da Quarta-feira de Cinzas". Composes the music "Canção do Subdesenvolvido" together with Chico de Assis.
- Composes score for the film, “Bonitinha mas ordinária” by Nelson Rodrigues”,