SCIV, although it was a tough decision:
The general cohesion it has wrapping all of the levels together and complimenting the settings, really shows the amount of work used in creating such a good feeling.
I also like how limited the resources were in comparision to SotN given they were released 6 years apart.
This does not detract my stance on SotN's soundtrack. Just comparing the two came down to how immersive the overall experience was.
However, ill have to agree with Intersection that LoI needs a place on this list as well.