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I think it's the shortened, nickname-style version of "Onii-san" (older brother in Japanese). I first heard it on Higurashi no Naku Koro ni, from the character Houjou Satoko. She called her older brother Satoshi "Nii-nii".

Younger children tend to use "Nii-Nii". It's a cute way to say "big brother".

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13y ago
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Q: What does Nii-Nii mean?
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