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Portal, but that one's already been mentioned.
Assassin's Creed's story was kind of nice in the end, but that game sucked for the biggest part.
If I had ever played Majora's Mask I would put it here, but I haven't (please Nintendo, put it on the VC)
I guess Half-Life, but that's more the feeling you get of it than the story.

But most of the games I play don't focus on the story but on gameplay, so I can't really say if something is as ''intellectual'' as Portal, or Grim Fandango :P

@Imperial: are you being sarcastic? Because I find it strange if someone who doesn't want to play ''smart'' games to be on a forum that's about statistics.