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If you don't mind old animation, then Nausicaa of the Valley of the Wind is a must.
Other anime that I think is excellent but doesn't get enough attention is Bokurano, Byousoku 5 Centimeter (maybe it's popular in this forum but not really anywhere else), The Place Promised in Our Early Days, Kino's Journey, SaiKano, and Seirei no Moribito (it has quite a bit of attention but not as much as it deserves).
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