Luiz Floriano Bonfá was born in Rio de Janeiro on October 17, 1922, to an Italian immigrant father, and grew up in Santa Cruz, on the rural western edge of the city. At eleven he began studying with the Uruguayan classical guitarist Isaías Sávio. The lessons meant a long weekly commute, a walk followed by about two and a half hours on the train, to Sávio's home in the hills of Santa Teresa, and Sávio taught him anyway when the family could not pay.

Bonfá reached a wide Brazilian audience in 1947, when he was featured on Rio's Rádio Nacional, and in the late 1940s he sang with the vocal group the Quitandinha Serenaders. His early songs "Ranchinho de Palha" and "O Vento Não Sabe" were recorded by the crooner Dick Farney in the 1950s, and his first hit as a composer, "De Cigarro em Cigarro," was recorded by Nora Ney in 1957. Farney introduced him to Antônio Carlos Jobim and the poet Vinicius de Moraes. Moraes's play Orfeu da Conceição opened at Rio's Theatro Municipal on September 25, 1956, with Jobim co-writing the songs and conducting and Bonfá playing guitar, and Odeon released the music on an LP the same year. His own recordings began with a 10-inch record on Continental in 1955 and continued mostly on Odeon through the decade. By 1957 he was dividing his time between New York and Rio, touring the United States with the singer Mary Martin and recording for American labels, among them ¡Amor! The Fabulous Guitar of Luiz Bonfa (Atlantic, 1958).

The turning point came in 1959, when the French director Marcel Camus asked him to contribute music to the film version of Moraes's play, released as Black Orpheus (Orfeu Negro). Bonfá wrote "Samba de Orfeu" and "Manhã de Carnaval," the latter with a lyric by Antônio Maria. Camus first rejected "Manhã de Carnaval," and Bonfá argued for it against a replacement he had written, and won. The film took the Palme d'Or at Cannes and the Academy Award for Best Foreign Language Film, and the song became one of the first bossa nova pieces to find an audience outside Brazil. Carl Sigman's English lyric turned it into "A Day in the Life of a Fool." That same year Bonfá recorded the solo album O Violão de Luiz Bonfá for Cook, which Smithsonian Folkways reissued in 2005 as Solo in Rio 1959 with previously unreleased material from the session.

His standing with American jazz players rose in 1962 and 1963. On November 21, 1962, the Brazilian Consulate General presented a bossa nova concert at Carnegie Hall, billed as the first North American concert of the style, with João Gilberto, Jobim, Bonfá, Roberto Menescal and Sérgio Mendes among the performers, a few months after Stan Getz and Charlie Byrd had started the American craze with Jazz Samba. A recording of the evening issued by Audio Fidelity credits Bonfá with a solo "Manhã de Carnaval" and, with the singer Agostinho dos Santos, who had dubbed the singing of Orfeu in the film, with "Manhã de Carnaval" and "A Felicidade." Verve, with Creed Taylor producing, recorded Luiz Bonfá Plays and Sings Bossa Nova in New York on December 30 and 31, 1962, with string arrangements by Lalo Schifrin, his wife, the singer Maria Helena Toledo, the alto saxophonist and flutist Leo Wright, and Oscar Castro-Neves. Jazz Samba Encore!, credited to Getz and Bonfá and produced by Taylor, was recorded in New York on February 8, 9 and 27, 1963, and released in April, with Jobim on guitar and piano and Toledo singing on seven of the eleven tracks. The record pairs three Jobim and Moraes songs, including "Insensatez" and "O Morro Não Tem Vez," with Bonfá pieces: "Sambalero," "Samba de Duas Notas," "Saudade Vem Correndo" and "Ebony Samba."

Bonfá worked steadily in the American pop and film market through the rest of the decade, and that work was as much a part of his career as the jazz dates. His song "The Gentle Rain," with lyrics by Matt Dubey, came from the 1965 film of that name, whose soundtrack he recorded for Mercury with Eumir Deodato, and Quincy Jones included it on Quincy Plays for Pussycats that year. He played guitar on "Samba de Orfeu" and "The Gentle Rain" for Tony Bennett's The Movie Song Album (Columbia, 1966). He recorded for Dot and RCA, made Stevie & Eydie, Bonfá & Brazil (Columbia, 1967) with the vocal duo Steve Lawrence and Eydie Gormé, played on American television with Perry Como and Caterina Valente, and wrote "Almost in Love," which Elvis Presley sang in the 1968 MGM film Live a Little, Love a Little. He played guitar on one track of George Benson's I Got a Woman and Some Blues (A&M, 1969), and Frank Sinatra sang "A Day in the Life of a Fool" on My Way (1969). On Jacarandá (Ranwood, 1973) Deodato arranged and conducted most of the tracks and the band included Idris Muhammad on drums, Stanley Clarke on electric bass, the conga player Ray Barretto and Airto Moreira on percussion.

According to AllMusic, his profile in the United States all but disappeared after the 1960s, though he kept touring and writing and eventually made more than fifty albums. In 1986 he was the special guest on Yana Purim's For a Distant Love, which also featured Airto, Patrice Rushen, Steve Swallow and Toninho Horta. American listeners met him again with Non-Stop to Brazil (Chesky, 1989) and The Bonfá Magic (Caju, 1991, issued in the United States by Milestone), the latter with Nilson Matta on bass and Gene Bertoncini on guitar, and in 1992 he was a guest on the harmonica player Toots Thielemans's The Brasil Project (Private Music), an all-star Brazilian program that included Lee Ritenour, Dave Grusin and Ivan Lins, playing guitar on "Manhã de Carnaval"; Wikipedia also lists him on its sequel. From 1990 to 1999 he worked with the singer Ithamara Koorax, who recorded Almost in Love: Ithamara Koorax Sings the Luiz Bonfá Songbook in 1996 with Bonfá on acoustic guitar and guests who included Larry Coryell, Deodato, Ron Carter, the percussionist Marcos Suzano and Sadao Watanabe; the sessions were filmed for a Japanese television program presented by Watanabe. He wrote scores for about two dozen films, among them 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, the last in collaboration with the arranger Hans Zimmer.

Bonfá passed away of cancer in Rio de Janeiro on January 12, 2001, at 78. He was then working on music for a film produced by and starring Karen Black and for a Broadway show about Carmen Miranda titled Brazilian Bombshell, to star Sônia Braga.

Bonfá is best known as a bossa nova and samba-canção composer and film-score writer, and much of his American output was pop-oriented rather than jazz. His jazz link is real and documented in three ways: the 1963 Jazz Samba Encore! sessions with Stan Getz, the Verve date with Schifrin and Wright, and the steady stream of jazz musicians who took up his tunes. Wikipedia's list of recordings of "Manhã de Carnaval" includes Wayne Shorter (Wayning Moments, 1961), Vince Guaraldi (Jazz Impressions of Black Orpheus, 1962), Getz (Big Band Bossa Nova, arranged by Gary McFarland, 1962), Quincy Jones, Ramsey Lewis (1962), Cal Tjader (1963), Paul Desmond (Take Ten, 1963), Gerry Mulligan (Night Lights, 1963), the Modern Jazz Quartet (1964), Dexter Gordon (Gettin' Around, 1965) and Charlie Byrd (1966), and Billy Eckstine and Astrud Gilberto recorded it as well.

As a player he was trained as a classical guitarist, and he brought a bold, lyrical, heavily orchestrated manner from the samba-canção tradition that came before João Gilberto's quieter bossa nova. Wikipedia describes his tone as brassier and more penetrating than Gilberto's, and notes that Bonfá was a frequent soloist where Gilberto was almost purely a rhythm guitarist. He often played solo guitar in a polyphonic style, harmonizing melody lines in a way comparable to Wes Montgomery, or playing lead and rhythm parts at once. His historical role was bridging the older samba-canção idiom and the new bossa nova. AllMusic lists his genres as Latin, International, Jazz and Pop/Rock, and his styles as bossa nova, Brazilian jazz, film score and fusion. Several of his recordings have since been sampled in hip-hop and electronic music, among them "Saudade Vem Correndo" and "In the Shade of the Mango Tree."