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Best atmosphere and level design by far; the places all really felt like locations and environments. At almost no point did I think, "This sure just feels like a pointless corridor." A feeling I got sometimes in DkS, and 99% of the time in DkS2.
I also have to submit a vote for best NPCs and their accompanying voice actors. Hearing Yurt in that cage, or Astraea requesting that you leave, are lines I will never forget.
The amors are also the best designed, albeit with their near futility in PvP.