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Certain memory access requirements by some mod installers, such as FROST or the System Shock 2 patcher, cannot be performed on a controlled folder. So, if a mod you're installing specifically says you need the game to be outside of Program Files (x86) to properly install, then you need to be outside of Program Files (x86) to properly install.
Alternatively, you could change Controlled Folder Access settings, but this isn't recommended. As minor as this protection scheme is, reducing its reach is an unnecessary risk when you could just install the game elsewhere.
Moving things is a fairly straightforward cut and paste operation. This video covers the how and why.
https://video.search.yahoo.com/search/video?fr=yfp-t&ei=UTF-8&p=gamerpoet+moving+a+steam+installation#action=view&id=2&vid=8919a5b04722d5c3ea2824d6ff30b5b4
I recommend watching the whole video, though the steps to move Steam when you only have a single installed drive begin around timestamp 2:10.
After moving Steam, if you are using a mod manager, LOOT, xedit, or any other tools, you will need to update all their settings to account for the new location.
You have the 25+ badge. At your library size, it's probably going to be the most convenient to just back up your games, uninstall Steam, then reinstall in the new location and restore the backups. Alternatively, if you have a second internal drive, just create a new library folder and have Steam move your games there, minus any older titles that don't play nice on a non-C drive (looking at YOU Wizardry 8).
EDIT: That said, you don't own FO4 on Steam. What version are you even playing?
https://support.steampowered.com/kb_article.php?ref=7418-YUBN-8129&l=
This^^ If your computer and your finances can manage it, putting your Steam, games, and tools on a second internal drive makes a lot of things easier.