I don't really see much point of tagging all their picture with that(even in their cat form) as I thought that tag would already be applied with them or something. It would be the same having them tagged as youkai. Or tagging all post that include Remilia_scarlet and Flandre_scarlet with vampire.
We already know what they are(or at least most of us) so it won't make too much of a difference.
But if it helps with simplier and/or better searching I'm not going to object.
Updated