In 1969, the group participated in V Festival de Música Popular Brasileira, playing the song 'De vera'. This song was on the band's first album, É ferro na boneca, recorded one year later. Initially their sound was a fusion of  with traditional folk sounds from Brazil.

Originally, the group only played with Pepeu Gomes and Jorginho at their live shows. However, gradually, Gomes started to acquire an ever more important role in the group: after he married Consuelo, he became a fully fledged band member and song arranger along with Moreira.

Their music began to gravitate more towards MPB, particularly due to 's influence, who frequently visited the group. Their second album  contained the classics 'Brasil Pandeiro', 'Preta Pretinha', 'Mistério do Planeta' and 'Besta é tu'. It was recorded on the Som Livre label in 1972, and years later would be considered the best Brazilian music album by Rolling Stone magazine. It was around this period that the group incorporated  as an auxiliary band.

In 1972, after recording Acabou Chorare, Novos Baianos moved to a community in , . In a garage where they lived they used to play, compose and play soccer. That was the reason for the name of their third album, Novos Baianos F.C., recorded on label Continental in 1973. The group had a strong  image at this time.

The band released records until their break-up in 1978. In 1974, they recorded the first album without Moreira, who decided to start his own solo career. As Moreira had previously composed songs with Galvão and arranged songs with Gomes for the bands previous albums, it was a great loss to the band. The members tried to continue and incorporated Gato Félix to the group.

In 1976, Dadi left the group to start a new band . Novos Baianos substituted Didi, the brother of Pepeu Gomes, for the loss of Dadi. However, the group disbanded some years later due to members starting their solo careers. Despite the end of the band, Novos Baianos' members reunited many times to celebrate special events.

In 1997, the composer of the group, Luiz Galvão, published the book Anos 70: Novos e Baianos for Editora 34. In the book he tells the history of the group and its importance to Brazilian music. After Galvão released the book, the group reunited to record a new album, named Infinito Circular, recorded live at Metropolitan, Rio de Janeiro. In 2007, Moreira also published a book about the group. It was written as a  and was named A História dos Novos Baianos e Outros Versos.

In 2009, the band reunited without Moreira to celebrate 40 years of Novos Baianos and their revolutionary role in Brazilian music. They also plan to record an album with an unreleased song.