I'd say either Hyouka, Uchouten Kazoku or Shinsekai Yori.
For nostalgia's sake (and I think it still holds up as one my favourite "children's" anime) I choose you, Digimon Adventure!
And probably the anime that really got me into anime and watching new series every season: Fumoffu, Haruhi and Toradora.
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Still remember racing home after school to watch 'Battle of the Planets'
https://www.youtube.com/watch?v=acOnskcyrtA
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Lupin III. It is old one, but stylish than recent animes.
https://www.youtube.com/watch?v=_1h4mQAEWI8
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Tough choice... but favourite is probably Perfect Blue or Princess Mononoke. Both exceptional films.
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