So, the results were good, especially on the cpu side of things, but now the GPU is pretty much back to normal temps I was seeing with the stock paste (after only one day). I have a feeling it could be the thermal pads were a bit too thick (1.5mm) on the VRAM which may be causing the heat sink to have limited contact with the GPU. I'm going to remove the pads and apply Kryonaut to the VRAM instead. I'll report back tomorrow with my results.
Ok! So I got my hands on some Hydronaut (couldn't find any Kryonaut) thermal paste and reapplied. The numbers are looking great! I was correct in my assumption that the thermal pads were not allowing the heat sink to properly sit on the GPU section on the laptop. That's probably why ASUS shipped this laptop with thermal paste instead of pads to begin with (I should have known).
In testing The Witcher 3 on high-ultra settings, before the repaste I was hitting 76-78 degrees. Now, 69-70!
I also noticed that someone else on this forum had a similar experience with their ROG laptop, check out the post by user Dimonic here
All in all, I'd say that applying thermal paste instead of thermal pads to the GPU VRAM and vrm of the CPU has made a huge difference for me!