Loved Valk Chronicles (which is number 2), but Id have to go with Demon's Souls without a doubt.
No other game this gen has had the emotional effect on me that DS has had :) The Game will make you sweat, curse, throw stuff, yell, cry, pull out your hair, and yet at the end of the day will just bathe you in utter satisfation for completing something that you deemed impossible when you started.
I equate Demon's Souls to my girlfriend. Whenever I screw up its ALWAYS my fault and never the games/hers.
Then there is NG+, which takes everything above x 4 (+ adds the thoughts of mass murder) and there you have it.