...a mod that overhauls the combat AI of NPCs so their behaviors more accurately reflect real opponents, instead of constantly running straight at you swinging a weapon while running unafraid juggernauts.
It's an older one, but I would highly suggest http://www.tesnexus.com/downloads/file.php?id=2073. It makes NPCs more likely to dodge, use power attacks, block or rush at you. I've found that it also seems to help in making NPCs more aware of their health, so they'll run away or back up if they think they might be getting weaker. According to the author's description, it also make guards much more of a challenge.
I combine this mod with MOBs and Kuertee's damage modifiers to get much more intense fighting situations. I tend to die a lot in my games, but it makes me feel like the NPCs are just as aware of what they're doing as I do. If you want to see the latter two together in action, I made a post and video about it for my blog. That would be the second link in my signature.