Lani Hall sang all the female vocals on Herb Alpert Presents Sergio Mendes & Brasil '66 except "Aqua de Beber" performed by Janis Hansen.

"Mas Que Nada" peaked at #4 on Billboard's Easy Listening chart on September 24, 1966.

In June 1967, Mendes' partner and manager, Richard Adler met with A&M sales and promotion personnel in London, Rome, Paris and Stockholm to discuss a concert tour of Europe.

In 1968, Sears refused to sell the Fool on the Hill album because it did not agree with the album cover art. The group is sitting on a woman's stomach and the back cover shows her nipple. In response, a sticker was placed over the nipple.

In February 1968, Mendes added Karen Phillip as the second vocalist and Sebastian Neto on bass.

In March 1968 Brasil '66 toured Japan. They returned for a second tour in March 1969. Also in 1968 was a six week tour of Brazil.

The single "Scarborough Fair" was among Australia's Best Sellers and was ranked #7 on March 15, 1969. It was ranked the #39 Top Single of the year in Australia in 1969.

Fool On the Hill was a #3 best seller in Japan in March and July 1969.

Lani Hall left the group in 1970. With her departure, Mendes reorganized the group by adding Gracinha Leporace, Claudio Slon on drums and Laudir De Oliveira on conga. Gracinha's first vocals with Brasil '66 were "Lost in Paradise" and "Chelsea Morning" on the Stillness album.

The group toured Australia in September 1970. Billboard reported airplay and record sales were at an all time high.

In late September or early October 1970, the group re-signed with A&M Records. The deal was a four-year contract.

"Scarborough Fair" was used in the 1973 film "Heavy Traffic."