Psychonauts definitely, because it has the insanity... of a manatee.
Also, although personally I would consider all of these adventures:
Appeal's Outcast: lose yourself in a wonderful alien world, then save it. Lots of story and character, a good bit of action with a touch of stealth and the strangest means of transportation ever.
Little Big Adventure 1 & 2: wonderfully charming. Overthrowing an evil dictator has never been this much fun.
Deus Ex: fascinating futuristic dystopia.
Gothic 1 & 2: it feels more adventure than RPG. Interesting story and characters, wonderful exploration and general awesomeness.
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