Wilson Simonal: Nem Vem que Não Tem
Though a seminal force in the development of Brazilian popular music, singer Wilson Simonal remains largely unknown outside of South America — the architect of the sound that dominated Brazilian charts during the late '60s, he was the nation's first black pop superstar, but his career never recovered from accusations that he was a police informant. Here's one of the highlights of his career from his 1967 LP Alegria, Alegria!!! but you'll have an easier time finding Gilles Peterson In Brazil from 2004.
Os Mutantes: Baby (1971)
Os Mutantes were one of the most dynamic, talented, radical bands of the psychedelic era — quite an accomplishment during a period when most every rock band spent quality time exploring the outer limits of pop music. Os Mutantes recorded Baby twice, once with some serious psychedelic fuzz guitar and organ in 1968 and this more mellow acoustic version from 1971 featuring Rita Lee on vocals. Find it originally on the LP Jardim Eletrico or more likely on the Luaka Bop release Everything Is Possible: The Best of Os Mutantes.
Raul Seixas: Metamorfose Ambulante
Raul Seixas was a fundamental rocker in Brazil. I have to admit I don't know too much about this recording but you can find it on many Brazilian compilations. I strongly recommend the City of God soundtrack from 2003. By the way the movie is great as well!