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Madoka (Faust the anime), Hell Girl (Shinto Faust the anime), Shiki (Greek Tragedy with vampires the anime), Shigofumi and Welcome to the NHK have the psychological down pat, but are light on the horror. From the New World (Though you need to give it time). Texhnolyze and Boogiepop Phantom (These two have the visual medium equivelent of a high reading age). Another is definitely psychological horror and a lot of people liked it. I didn't, but then again I didn't like Elfen Lied much either.
If you dare to dabble in the world of visual novels, the Higurashi visual novel is much more psychological and in depth to start with, then by the same author there's also Umineko. Corpse Party has been available legally a few years and also has an anime adaptation which isn't bad but is by no means spectacular. Saya no Uta is the elephant in the room here (I can't be held responsible for the content or your reaction to it) and Tsukihime is an old classic for a reason.
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Thanks! I'll start checking these out. Sayu no Uta sounds really interesting. From what I've read it seems like exactly the type of thing I'm looking for, sort of Jacob's Ladder/Silent Hill 3-esque, visually, of course. I've become really desensitised to horror in general, the only thing that still gets me is videogames, so I'm hoping this will.
For now I think I'm going to start with Madoka and Another.