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What did it for me was do exactly this but in the "Change settings for all users." That kinda...locked it in.
Man thank you so much for this thou! Somehow I got to play two older games at the same time that BOTH have this issue! Other being FF13 Lighting Returns, in that game I just assumed its game having bad AA or something since it just looked kinda blurry. BUT NO! It's exactly same issue as with Call of Cthulhu, now both game looks great! Kinda new to 4K at this point but planning on playing lot of older games so this is EXTREMELY good thing to keep my eye out if resolution seems to be not quite right. I bet there is ton of games with this quirk.
You have to click on "Properties" after right-clicking the .exe file. After that you go to the compatibility tab and follow the rest of the guide.
I have now updated the guide to include the missing step.
Try going into Windows settings, System, Display, Scale and Layout and change the option under "Change the size of text, apps and other items" to 100%.
This might make everything on your Desktop look too small, but try booting into the game like that. That's the only idea I have if the above didn't help.