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I'm actually going to pick episode 2.
Day of Sagittarius, and Live a Live are pretty much tied for a close 2nd for me, but I've always felt that the quality of a work's (true) beginning and the quality of a work's (true) ending are of particular importance.
Episode 2 really made the Haruhi universe come to life for me, particularly due to its art style, animation quality, and overall creative direction. The episode managed to blend the surreal nature of many of its primary characters with a nonetheless very realistic setting and a practical touch-point character in Kyon.
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