Graphical/textures/meshes, interface, bugs... I grabbed the game in the Steam sale and I'm looking to pimp and smooth it out before starting. Something that makes the UI bearable would be nice, similar to Sky UI or Immersive HUD. Higher poly player and world meshes would be nice, too, as well as better environment textures.
So far I've downloaded the Updated Unofficial Fallout 3 Patch, NMCS Texture Pack, An Eye Improvement Mod.