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It still sounds rather like it may be a permissions matter, however, it may acting correctly in preventing access to Calibre. Even though you can manually add files to your C:\Calibre directory with File Explorer it still may be that security is preventing an application (such as Calibre) from doing so. Windows 8 is stricter on C: drive security than previous versions.
The easiest way to test this without getting involved in changing the C: drive's default permissions is if your drive is partitioned to have a D: (or other) drive, then just try moving your library onto that to see if that solves it.
If your drive is not partitioned then try putting your library into your user account's area of C:\Users\username\... , preferably in Calibre's default library folder (sorry I do not recall what that is, I have always kept my libraries off the C: drive, but should be easy enough to determine or someone will advise). C:\Users\... is where applications are supposed to write to if they wish to write to that drive.
Alternatively, if your drive is not partitioned, you could just try copying the library to a USB stick or drive and select that as the library from within Calibre and see if it works. If that works then easiest is to then move your library into C:\Users... as described above, and where it should still continue to work.
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