This is exactly what I was about to suggest, with the added comment that since OSX follows aliases even INSIDE disk images (found that long ago, don't remember if a hint was posted already), this method should work in yet unsuspected situations. Like, maybe, keeping the existing users folders where they are but replacing their subfolders with aliases pointing inside disk images elsewhere (allowing distinct quotas for Music and Documents? Easing backup of users stuff? Combine with "real" quotas to minimize usage of the boot volume and store user data to other locations?)

I'm not sure how well this would work, but it seems worth trying.

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