Buarque came from a privileged intellectual family background—his father Sérgio Buarque de Holanda was a well-known historian, sociologist and journalist and his mother Maria Amélia Cesário Alvim was a painter and pianist. He is also brother of the singer Miúcha. As a child, he was impressed by the musical style of bossa nova, specifically the work of Tom Jobim and João Gilberto. He was also interested in writing, composing his first short story at 18 years old and studying European literature, also at a young age. One of his most consuming interests, however, was playing soccer, beginning at age four, which he still does today. Though he was born in Rio de Janeiro, Buarque spent much of his childhood in Rio de Janeiro, São Paulo and Italy.

Before becoming a musician, Buarque decided at one point to study architecture at the University of São Paulo, but this choice did not lead to a career in that field; for Buarque often skipped classes.

He made his public debut as musician and composer in 1964, rapidly building his reputation at music festivals and television variety shows when bossa nova rhythm came to light and Nara Leão recorded three of his songs. His eponymous debut album exemplified his future work, with catchy sambas characterized by inventive wordplay and an undercurrent of nostalgic tragedy. Buarque had his first hit with "A Banda" in 1966, written about a marching band, and soon released several more singles. Although playing bossa nova, during his career, samba and Música Popular Brasileira would also be widely explored. Despite that, Buarque was criticized by two of the leading musicians at the time, Caetano Veloso and Gilberto Gil as they believed his musical style was overly conservative. However, an existentially themed play that Buarque wrote and composed in 1968, Roda Viva ("Live Cycle"), was frowned upon by the military government and Buarque served a short prison sentence because of it. He left Brazil for Italy for 18 months in 1970, returning to write his first novel in 1972, which was not targeted by censors.At this time his thinly-veiled protest single "Apesar de Você" ("In spite of You" --in reference to the military dictatorship)was also produced. ("In spite of you") was overlooked by the military censors, becoming an important anthem in the democratic movement. After selling over 100,000 copies, the single was eventually censored and removed from the market. At one point in 1974, the censors banned any song authored by Chico Buarque. Then, he created a pseudonym, naming himself "Julinho da Adelaide", complete with life history and interviews to newspapers. "Julinho da Adelaide" authored songs such as "Jorge Maravilha" and "Acorda amor" before he was outed in Jornal do Brasil news story. Buarque also wrote a play named Calabar, about the Dutch invasion of Brazil in the seventeenth century, drawing parallels with the military regime. Despite the censorship, songs such as "Samba de Orly" (1970), "Acorda amor" (1974, as "Julinho da Adelaide") manifested Buarque's continuing opposition to the military regime.

During the 1970s and 1980s, he collaborated with filmmakers, playwrights, and musicians in further protest works against the dictatorship. Buarque approached the 1983 Concert for Peace in Nicaragua as a valid forum to vocalize his strong political views. Throughout the decade, he crafted many of his songs as vehicles to describe the re-democratization of Brazil. The Concert for Peace in Nicaragua was one in a concert series known as the "Central American Peace Concerts." These concerts featured various Latin American artists. The political turmoil that plagued this era were expressed in many of Buarque's songs. He later wrote Budapeste, a novel that achieved critical national acclaim and won the Prêmio Jabuti, a Brazilian literary award comparable to the Man Booker Prize.

During Brazil's military coup d'état of 1964, Buarque wrote about the events which transpired and avoided censorship by using cryptic analogies and wordplay. For example, in the song "Cálice" ("Chalice", or Jesus' Last Supper "Cup"), a duet written and performed with Gilberto Gil, he takes advantage of the homophony between the Portuguese imperative "shut your mouth" --cale-se-- and "chalice" --cálice-- to protest censorship against freedom of speech by the dictatorship, disguised as the Gospel narrative of Jesus' Gethsemani prayer to the Father to pass from Him the chalice of bloody death probation. The line "I wanna sniff diesel fume" is a reference to the death of political prisoner Stuart Angel, who had his mouth glued to a jeep's exhaust pipe during a torture session. Buarque was a friend of his mother Zuzu.

• 1966: Chico Buarque de Hollanda (Vol. 1)
• 1966: Morte e Vida Severina
• 1967: Chico Buarque de Hollanda (Vol. 2)
• 1968: Chico Buarque de Hollanda (Vol. 3)
• 1969: Umas e outras - compacto
• 1969: Chico Buarque na Itália
• 1970: Apesar de você
• 1970: Per un pugno di samba
• 1970: Chico Buarque de Hollanda (Vol. 4)
• 1971: Construção
• 1972: Quando o carnaval chegar
• 1972: Caetano e Chico juntos e ao vivo
• 1973: Chico canta
• 1974: Sinal fechado
• 1975: Chico Buarque & Maria Bethânia ao vivo
• 1976: Meus caros amigos
• 1977: Cio da Terra compacto
• 1977: Os saltimbancos
• 1977: Gota d'água
• 1978: Chico Buarque

• 1979: Ópera do Malandro
• 1980: Vida
• 1980: Show 1º de Maio compacto
• 1981: Almanaque
• 1981: Saltimbancos trapalhões
• 1982: Chico Buarque en espanhol
• 1983: Para viver um grande amor
• 1983: O grande circo místico
• 1984: Chico Buarque (Vermelho)
• 1985: O Corsário do rei
• 1985: Ópera do malandro
• 1985: Malandro
• 1986: Melhores momentos de Chico & Caetano
• 1987: Francisco
• 1988: Dança da meia-lua
• 1989: Chico Buarque
• 1990: Chico Buarque ao vivo Paris le Zenith
• 1993: Para Todos
• 1995: Uma palavra
• 1997: Terra

• 1998: As cidades
• 1998: Chico Buarque da Mangueira
• 1999: Chico ao vivo
• 2001: Chico e as cidades (DVD)
• 2001: Cambaio
• 2002: Chico Buarque — Duetos
• 2003: Chico ou o país da delicadeza perdida (DVD)
• 2005: Meu Caro Amigo (DVD)
• 2005: A Flor da Pele (DVD)
• 2005: Vai passar (DVD)
• 2005: Anos Dourados (DVD)
• 2005: Estação Derradeira (DVD)
• 2005: Bastidores (DVD)
• 2006: O Futebol (DVD)
• 2006: Romance (DVD)
• 2006: Uma Palavra (DVD)
• 2006: Carioca (CD + DVD with the documentary Desconstrução)
• 2007: Carioca Ao Vivo

Books

• 1966: A Banda (Songbook)
• 1974: Fazenda Modelo
• 1979: Chapeuzinho Amarelo
• 1981: A Bordo do Rui Barbosa
• 1991: Estorvo
• 1995: Benjamin
• 2003: Budapeste
• 2009: Leite Derramado

Plays

• 1967/8: Roda Viva
• 1973: Calabar (coauthored with Ruy Guerra)
• 1975: Gota d'água
• 1978: Ópera do Malandro (based on John Gay's Beggar's Opera and Bertolt Brecht's Threepenny Opera)
• 1983: O Grande Circo Místico

Film

• 1972: Quando o carnaval chegar (coauthor)
• 1983: Para viver um grande amor (coauthor)
• 1985: Ópera do Malandro
• 2009: Budapeste (based on his book)