It was through Farney that Bonfá was introduced to Antônio Carlos Jobim and Vinicius de Moraes, the leading songwriting team behind the worldwide explosion of Bossa Nova in the late 1950s to 1970s, becoming a fever in the US.

Bonfá wrote some of the original music featured in the film, including the numbers "Samba de Orfeu" and his most famous composition, "Manhã de Carnaval" (of which Carl Sigman later wrote a different set of English lyrics titled "A Day in the Life of a Fool"), which has been among the top ten standards played worldwide, according to The Guinness Book of World Records.

Jobim, João Donato, Dorival Caymmi, and other contemporaries were also essentially samba-canção musicians until the sudden, massive popularity of the young Gilberto's unique style of guitar playing and expressively muted vocals transformed the genre.

From 1990 to 1999, Bonfá worked with singer Ithamara Koorax on several recordings and concerts, appearing live with her as special guest at several venues in Rio de Janeiro such as Teatro Rival, BNDES Auditorium and Funarte-Sidney Miller Hall.

Bonfá wrote soundtracks for two dozens of movies, such as Black Orpheus, O Santo Módico, Os Cafajestes, The Gentle Rain, Pour Un Amour Lointain, Le Ore dell'Amore, Carnival Of Crime and Prisoner Of Rio (on which he collaborated with arranger Hans Zimmer), among many others.

In 2008, Universal Music France released a coffee table book containing two CDs which included previously unreleased material of the Black Orpheus soundtrack, and a DVD.

Bonfá's major legacy continues to be his compositions from the Black Orpheus soundtrack, most notably the instantly recognizable bossa nova classic "Manhã de Carnaval".

Japanese DJ Nujabes ヌジャベス also sampled "Shade of the Mango Tree" (from 1980's Bonfa Burrows Brazil) in his track "Lady Brown" on the album "Metaphorical Music" in 2004.