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So, is there anything else out there which even comes close to the wonderful high-fantasy worlds of Last Exile and Simoun?
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Since when Last Exile and Simoun are fantasy? Last exile especilly is full of relatively advanced technology, not magic. It is science fiction and Simoun also is more science-fiction than fantasy, IMO. Maybe you mean fantasy/sci-fi with an interestingly developed setting/world? If yes:
Juuni Kokuki
Full Metal Alchemist (the plot and characters of this series are overrated, IMO, but the setting is well developed)
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As a consolation prize, since I'm currently basically only watching Toku and action/mecha anime, I'm also possibly looking for anything else that has similar excellent character drama and plot
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Planetes
Mai-HiME (it's deceptively light-hearted and funny at first, though)
P.S. When I saw the title of the thread I thought you were looking for series with air battles and no giant robots but I guess I was wrong.