If you liked
Koukaku no Regios
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...then you might like
Shuumatsu Nani Shitemasu ka? Isogashii desu ka? Sukutte Moratte Ii desu ka?
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Both main leads were from orphanages, they were the older-brother figures in their respective orphanages. Both are set in a post-apocalypse world, both feature floating cities and its inhabitants fighting against monsters left on the uninhabitable surface. Both feature main female leads [Nina Antalk in Chrome and Chtholly in Sukasuka] prominent in the first half or so, but at the end overtaken by another female lead [Felli in Chrome and Nephiren in Sukasuka]
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Recommended by Matchamegu