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This was a tough one. But I’m probably going to have to say JSawyer Ultimate for Fallout: New Vegas. A continuation of the game director’s own rebalance mod, it makes the game hard in a way that feels fresh and fair (unlike the baked-in Hardcore mode).
I like to pair it with my runner-up: JAM - Just Assorted Mods, for a more modern HUD and a sprint feature. Of course then you need the NPCs Sprint mod to rebalance combat and- you know what, all of the Viva New Vegas modlist while you’re at it ;)