If your calibre library is very small, or you're willing to do it in lots of small steps :-)
You can select up to 50 books, and select from the context menu: Goodreads -> "Add to shelf..." (any shelf in Goodreads), but GR limits the amount you can hit the API, so you can only do 50 books at a time.
Alternatively, you dump your calibre books to CSV and add them right from the Goodreads website.
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