Good start. I only just did the large address space change, and it has completely fixed CTDs (I also have the game installed under my user directory, which itself fixed problems, too).
First, get FOSE and FOMM.
Fellout. It removes the haze over the game, and makes nights
dark. Night combat is exceptionally wild and suspenseful with this mod, and it fits the game's mood well. You definitely want to get your monitor's brightness, contrast, and gamma set right, though (if it has an sRGB option, just use that and be done with it), or you might end up seeing even less than intended at night.
Street lights, and
another.
DC Interiors. All fluff, but good fluff.
Auto-aim fix 1.1. The game aims for you. Just disabling it makes aiming a PITA, as it will no longer reliably aim towards the crosshair at all. However, by default, it will aim for body parts you aren't aiming for, including some that have cover. When sniping, you will notice that the projectile goes well above the crosshair after a certain distance, too. This mod, which just sets a few variables, makes the auto-aim zero at a very far distance, and only target what's right under the crosshair. If you have experience playing FPS games, don't even bother trying to play w/o this, or a similar, mod; you will just frustrate yourself, trying to deal with that buggy console+gamepad holdover.
Mart's Mutant Mod. I have all the new enemies turned off, and use it just for the wasteland spawn and encounter options.
Experience control book. The game, by default, gives way too much XP.
DUI (Darnified UI): very nice interface mod. Among other things, you can ditch most of the 10-ft interface stuff. You could try the Pipboy Readius, too, but I couldn't get it working right.
