So many cool suggestions in the comments, I have to add a mention of Ennio Morrricone’s soundtrack to “The Thing”.
On a personal note, Shnitke’s Concerto Grosso #1 always sounded like a manic bad dream to me.
Threnody to the Victims of Hiroshima
A warning to those who experience frisson or have high empathy experiences when listening to music - this is uncomfortable. There is a beauty to it, one that is drawn from the very dissonance and frenetic energy in it, but it’s a piece that is meant to make you grapple with discomfort.
Nick Cave - Tell Me What That Is from the Wind River soundtrack. It’s more sad and unsettling once you know the context and what happens in the film.
I had this discussion with a class the other day. It doesn’t answer your question really, but the Requiem for a Dream soundtrack is rather unsettling if you’ve seen the film.