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When you start Calibre up in the second user you can click on the Library icon on the toolbar to switch to the library that you want to share. This will then become the default library the next time you launch Calibre from that user. Note that you need to make sure that file permissions are correct for this second use to have full read-write access to the Library folder and all it's contents.
Use Preferences are stored on 'per user' basis which is why when you first start up Calibre in a new user it will not already be pointing to the library you set up under the previous user.
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