In my opinion, Fallout without question. The writing and the world itself in Fallout are immersive and intriguing. It manages to avoid some of that generic feel that comes with some elements of the Elder Scrolls franchise. I especially love the different factions and companions.
I just really enjoy the atmosphere, as well. It has the 1950's feel, with lounge singers and jingoistic propaganda, but combined with some outlandish, Jules Verne-type technology. I cannot wait for Fallout 4.