Thanks for posting the link to the map, very interesting. I'm intrigued that the Census specifically cites Moulds Level as the place of residence; the nearest village, Langthwaite is less than a mile away, and there are several farmsteads in the vicinity; the uplands had a greater population than today, so the census has really pinpointed a locality.
Moulds mine shop is shown on the map where you'd expect, adjacent to the level (where the tram lines converge), although nothing remains today, but the level itself. The mine shop is shown as significant structure, so your ancestor(s) may have resided there, at least temporarily.
The only other buildings in the immediate vicinity appear to be crushing mills, so would unlikely be dwelling-places.
As with so many other mining districts, there was both indigenous and itinerant populations. Surnames can often give us a further clue to their origins.