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All you can do is remove the game from your account, this way you'll be able to use his copy with DLCs.
And if not, how do i "remove" Dark souls 3 from my account?
Click on DS3 in the library > Click "Support" under Links on the right > "I want to permanently remove this game from my account"
Do keep in mind that you won't be able to play DS3 while your brother is playing any other game, unless he goes offline.
Family sharing DLC won't work if you have the base game. In any game.
//edit: Here, from the FAQ:
https://store.steampowered.com/promotion/familysharing