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nearly all relevant Bob Dylan material from the 60s has been offically released, see: Bootleg Series vol. 1-3 Bootleg Series vol. 4 (live 66 Manchester Free Trade Hall "Judas") Bootleg Series vol. 6 (live 1964) Bootleg Series vol. 7 ("No Direction Home" - 2 CDs accompaning the movie) and some more songs are on "Biograph" (released in 1985)
forget to mention that there are some unrelased live recordings from 1965-66. But you donĀ“t need them - unless you are not a diehard Dylan fan (and if you are, you already have them !)