Lot of great picks but I got to go with Castle of Cagliostro mainly because I'm a huge Lupin the 3rd fan but it's also legit beautifully animated. Plus it has some amazing action set pieces that quite a few other cartoons and movies have paid homage to. That episode of Batman The Animated Series featuring the Clock King is pretty much inspired by the climax of Castle.
A few honorable mentions for Princess Mononoke, Grave of the Fireflies, Perfect Blue, and Golgo 13: The Professional.
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