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Any books imported into calibre from your Kindle are in your library like any other books. You must give calibre access to those books, though, to import them, so it will not be automatic. What you CAN do, is tell calibre, in Preferences ==> Import/Export ==> Adding Books, in the Automatic Adding tab, to watch your Kindle for PC folder and automatically add all books from there. Then just download all books to Kindle for PC and they will be added. Or whenever you buy books, select deliver to K4PC.
You can also just add all the books that are not already in calibre when you plug in your Kindle. It is easy to tell which those are, since calibre will match all books as on device.
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