I can load the game, I can change my options without it crashing, but when I hit "new game" and watch/skip the intro video, it crashes.

Playing on Windows 10

I know I'm late to the thread but try this at the 'Crashing on New Game' section:

https://www.reddit.com/r/FalloutMods/wiki/fixguide

Good stuff. I scrolled down to the 'Crashing on New Game' section and installed the dsd9 fix for Nvidia. It seems to be working now, but I've encountered an old bug where the animation flips out when aiming with a gun. Gonna play around with the settings to see if I can get it to stop.