I believe Fate/Stay Night (Fan Translation) for the PC: 101 hours, 2 minutes, and 8 seconds, by kireev2000. The largest in terms of memory size I believe is Lego Batman for the PC, 2656256MB, by Geekmeister.
Fate/Stay Night is a visual novel, I personally don't consider visual novels as video games and think they shouldn't have a place in longplays.org. The longest video game longplay is EverQuest 2 (84 hours), which for some reason is missing from youtube from parts 04 to 35.
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