I have always enjoyed the stories where things become a bit mystical in Fallout.
Cabot House, Swamp People, The Interloper, etc.
Personally, I think it would be extremely fun to play a game where you hunt down clues and what not to search for an eldritch being. It would open up so much more lore and depth to the fallout world.
Anywho, thanks for listening to the ramblings of a crazy man.