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"Faust Wakes Nosferatu" is pretty amazing, and the vinyl is in an awesome tri-fold book package.
Faust IV and the Neu! catalogue form the basis for pretty much the entire early Stereolab musical style.
Others I love:
Witthuser and Westrupp
Agitation Free
Cosmic Jokers
Guru Guru (first three LPs are incredible)
Necronomicon (more German heavy prog then Krautrock per se, but from the same time period. "Tips Zum Selbstmord" is an absolute classic of heavy prog evilness)
The "Tone Float" album by the pre-Kraftwerk, Pre-Neu! collaboration known as Organisation is beautiful.
Popol Vuh made some incredible LPs as well, especially the soundtrack to Herzog's "Aguirre."
Ash Ra Tempel's first album is essential, as is the first album by Gila.
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