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Both of you need to check to make sure your accounts are not compromised in any way, as well.
And neither of you are using a VPN that might put one of the IP addresses in a different region?
These might seem silly questions, but I can family share my main account with my daughter, but I can't share my secondary account with my main on the exact same PC. After much testing, I found it's because of the store region mismatch and could consistently recreate a temporary fix.
If the store regions on both accounts are not the problem for the two of you, it might still be easiest to solve while you're both in the same physical location. So I'd suggest getting your PCs in the same room so you can each log into your accounts on the other's PC, and test from there.
Edited to add - I see a list of accounts under this setting (not the Manage Other Computers one) that I have to tick the box next to...
All you can do is setting it up from the start again, disable all authorizations and Family Share first and restart Steam, then go through the process from the start, you login to your brothers PC with your account and activate Family Share in the client settings, then he does the same on your PC.
Then restart Steam and see if it worked. Its a pain in the ass but often the only way to fix problems with Family Share.