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Rather than do that through Calibre, I prefer to Google book cover images myself. That way I can hand pick one of the appropriate dimensions and quality, download it and tell Calibre to use it via Edit Metadata > Change cover > Browse.
Doing it that way, I was able to replace the covers of all my Iain M Banks books with the same style of cover. Also I was able to substitute all the Harry Potter covers with the rather classy looking "adult" versions.
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