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AFAIK calibre doesn't offer what I think you asked for: a 'system generated' VL of books not in any other VL.
You could probably do it via a composite column (i.e. one built from other columns). I'll call it #notinanyvls. The column template would interrogate the list of VL's for which a book 'qualifies', if the list is empty it would set #notinanyvls to true. You'd define a VL Not in any VL with search expression #notinanyvls:true.
The Tutorials section of the calibre user guide has extensive doco on calibre's Template language.
BR
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