- Records two LPs, "Pobre Menina Rica" and "Sound of Ipanema", the latter with Paul Winter.
- “Pobre Menina Rica” opens at the Teatro Maison de France, starring Nara Leão, Napoleão Muniz Freire and Carlos Lyra, directed by Domingos de Oliveira.
- “Pobre Menina Rica” reopens at the Teatro de Bolso Aurimar Rocha. Cast includes Cléa Simões, Noriel Vilela, Milton Gonçalves, Ary Toledo, Roberto de Cleto, Vera Gertel and Carlos Lyra. Music performed by Antonio Adolfo’s group, “Trio em 3D”.
- “Aruanda” becomes “Take me to Aruanda” with lyrics by Norman Gimbel, and is Lyra’s first song to receive an English version.
- Children’s musical, "O Dragão e a Fada", receives the award from the State of Guanabara.
- First original songs in English: “It only could happen with you”, lyrics by Norman Gimbel and “A certain sadness”, lyrics by John Court. The latter is recorded on an LP released on the Verve label, sung by Astrud Gilberto.
- Score for the film, "O Padre e a Moça" receives awards as best film score for 1965 and 1966.
- Score for musical, "A Pobre Menina Rica", written with Vinícius, receives award for best musical composition for theatre.
- LP “Carlos Lyra” is released on the Capitol label in Mexico.
- Composes music for “The Song of Songs” from the Book of Solomon, performed in a recital at the National Library of Mexico, Mexico City.
- Composes music for the play, “La cueva de Salamanca” by Don Juan Ruiz de Alarcón, staged in Mexico City, directed by Hector Mendoza.
– Composes scores, writes text and does narration for 20 short subject films aimed at the tourist trade in México City during the Olympic Games.
- Musical "Pobre Menina Rica", translated into Spanish by Gabriel Garcia Marques and Mexican poet, Francisco Cervantes, opens in México. Cast includes Lyra (in the role of the Beggar Poet), Leny Andrade, Marly Tavares, and the Trio Bossa Três (Luis Carlos Vinhas, Rony Mesquita and Otávio Bailey).
- Composes songs for the play, “Fuenteovejuna” by Lope de Vega, staged at the Teatro Tlatelolco in Mexico City, directed by José Luiz Ibañez.
- LP “Saravá” is released in México on the RCA label.
- A version of the musical, Pobre Menina Rica, is produced for Mexican television with Kate Lyra in the title role.
- Produces and directs children’s musical, “O dragão e a fada”, at the Teatro de la Danza, in Spanish version, “¿Alguién dijo Dragon?”. Play receives awards for Best Direction, Best Cast, Best Musical Score, Best Sets, Best Costumes, recebendo and Best Musical Play.
- Returns to Brazil.
- Records "...e no entanto é preciso cantar", released on the Philips label with arrangements by Théo de Barros, and special participation of Kate Lyra and Chico Buarque de Hollanda. Chico and Carlos sing the first Buarque/Lyra song, “Essa passou” .
- Composes music for the play, “Abelardo e Heloisa” (a medieval drama of the Twelfth Century), staged in São Paulo and Rio de Janeiro, directed by Flávio Rangel.
- “Carlos Lyra – História da Música popular brasileira”, combination LP / booklet, released by Abril Cultural Publishing.
- LP "Eu & Elas", including first song written with Ruy Guerra, “Entrudo” released on the PolyGram label.
- "Pobre Menina Rica" opens at the Teatro da Praia. Cast includes Kate Lyra (in the title role) and Carlos Lyra.
- Records LP "Carlos Lyra", released on Continental label.