Without a doubt, Deadly Premonition.
It's a great game, it's just that it has very little replay value.
You see, on the first playthrough I wasn't bothered by the clunky combat or occasionally shoddy visuals. I was so engrossed in the story and characters that I didn't notice. In the ridiculously long driving sections, I'd often ponder who the killer really was, and I was genuinely stumped. I usually figure these things out, but I couldn't with Deadly Premonition.
The whole plot was brilliantly written, and as a Twin Peaks fan I loved all of the little shoutouts. It's a shame that the magic isn't as powerful the second time around.
Oh, and Bioshock would be good with that, becuase it also had a great plot twist. It was like the Polito/SHODAN thing but doubled.
Actually, if ANYTHING, I'd love to have read Dr. Jekyll and Mr. Hyde without any prior knowledge of it. Just think about how shocking the whole "Jekyll and Hyde are the same man" plot twist would be if you didn't already know it. Unfortunately, thanks to, well, everything, it's about as shocking as the assasination of Julius Caesar (in the play, that is) or the sinking of the Titanic (in the movie, that is)