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I recommend Grave of the Fireflies also.
However, I do think you should check out Now and Then, Here and There (Licensed). In a similar fashion to Narutaru, the first few moments could trick you into thinking it was a light-hearted anime. Also has semi-cutesy designs. But then it shifts into a really depressing atmosphere, and when I saw it, I was very thankful that I wasn't in the main character's shoes. It has an excellently crafted psychotic villain, who you will end up really hating. The plot isn't hard to follow (also deals with issues such as rape and child labour, amongst a few), the music is brilliant, and you'll probably want to watch the whole thing in one go. Please do consider buying this anime.
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