I am not a developer. But I must say, the UI really has quite some room for improvement, and luketheobscure, the direction you are suggesting with your designs makes it look a lot more usable.
Quite a lot of feature in calibre i tend to avoid (eg managing tags) because the UI is too cluttered in some aspects.
I think input from someone with UX skills like yours could really help the project! Just don't focus too much on the OSX design paradigms and try to have the rest of the userbase in mind.
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