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Check whether there are .ini files in Documents\My Games\Fallout4.
If this is not it then check your window scale.
Read here for more info, please:
https://steamcommunity.com/sharedfiles/filedetails/?id=3241230342
Before I made this post I actually went thru your post step by step in hopes to find a solution but none of the things you provided works for me for some reason. The Prefs.ini does exist, I set the resolution in there and in the installation folder to match 1 for 1, checked that the Controlled Folder Access is off, window scale is set to 100%, even the override to "Application" isn't doing anything. Changing the resolution to lower one and trying to scale it up with AMD Super Resolution also seems to do whole bunch of nothing (scales it up maybe a notch but still not as close to fitting the whole screen).
There actually was a line that was 0 but changing it to 1 didn't help.