For the family? "Castle In the Sky" and "Kiki's Delivery Service," as well as "Spirited Away" for the ones who can handle PG. All three are by Miyazaki, the guy who did "Princess Mononoke."
For the grownups, "Trigun" and "Cowboy Bebop" are two good ones to start with--keeping in mind that they're TV series, so you're in for several hours of watching.
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