Fallout New Vegas is the definitive Fallout experience. The Mojave Wasteland's gritty yeehaw vibe is unmatched, while an Obsidian at the height of its powers has yet to be bested in terms of writing wizardry within the series. It's a complete RPG in every facet, and would be my dream pick for a remaster, especially now Obsidian and Bethesda operate under the same umbrella. This, of course, would be years away, but the good news is that you can leverage modern graphics settings in the existing version of New Vegas right now.
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