I think most of my favourites have already been mentioned but here I go...
Caetano Veloso - Caetano Veloso (the one with "A Little More Blue" and "London, London"), "Transa" and "Araça Azul"
Gal Costa - Gal
Novos Baianos - Acabou Chorare
Os Mutantes - Os Mutantes (first album)
Los Hermanos - 4
Lula Cortes E Ze Ramalho - Paebiru
...