For Starters, ELDRITCH HORROR is probably my favorite game of all times. I'm a little bit biased on some of the new stuff in MOUNTAINS OF MADNESS, though, for example Preludes or new Sideboards I don't care about. Usually I just take the new stuff to pimp my vanilla-game, without having to change too much.
I had this idea for a completely optional small-box Expansion which would only add some cards to existing decks, with the goal of making the game harder and more challenging: these cards would include Tests, which would require at least 2 Successes on rolls in order to be counted as a success. Or give you different results, whether you have rolled 1 or 2 successes: for example, when resolving a "failed"-result on a complex encounter 1 success would be enough to get you alive without gaining anything, while 2 successes would still get you a consolation prize.
There shouldn't have to be a lot of them, just a couple to make a little bit more scared. Maybe 2 additional research-accounter for each (existing GOO), and some more Location/Generic Encounters and Other World Encounters. And maybe add to existing Spells and Conditions, 1 additional card per type, with a particularly more nasty backside effect.