After thinking about this some more, I have come to the conclusion that, regardless of what I do on CC, I have to move the books out of the unread pile on the Kindle. So, completing a book on the Kindle, I will move it to Read. Reviewing a book on CC that I decide to put off reading, I will move it to Defer on the Kindle. I suppose I should also have a Collection on the Kindle for books I decide I never want to read. Then, when I next sync the Kindle and Calibre, I will update the status in Calibre of books in those three collections and then delete Read and Won't Read from the Kindle. A bit clunky, but we'll see.
My wife replaced her Nook with an Android reader so that she could find books to read with CC. That is clearly simpler, but I really like the e-ink screens and the size and weight of the Kindle.
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