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Don't keep the calibre library in the user (\Users\whoever) or Documents folder (My Documents) because they change when you switch users. Instead put it in a dedicated folder somewhere (e.g., C:\MyLibrary) that both users can see. Move the library using one user. Shut down calibre, switch to the other user, and use calibre's Switch Library command to open the library at the new location. From this point on both users will see the same library.
As eschwartz says, do not run calibre on the same library as different users. Bad things will happen. This means that you can't use the tray icon, and you must explicitly stop/shut down calibre before you switch users.
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