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Reboot both the NAS and your computer. If you are using Windows, reboot the computer in safe mode with networking. Then without starting calibre, copy the library from the NAS to a local disk. Reboot in normal mode if needed, then use calibre to open the local library. Immediately run calibre's "check library" to see what damage you are facing.
If calibre can't open the local library then try to rebuild it, as you apparently already tried to do with the NAS copy.
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