Hello Ford, Edward,
As per the description, we understand that you want to block IPv4 address to your mailboxes.
I request you to sign-in to Defender portal at https://security.microsoft.com
Navigate to Email & collaboration > Policies & rules > Threat Policies > Rules section > Tenant Allow/Block Lists.
Here you can add your IPv4 address which you want to block in the block option as shown in the below screenshot.
If you manually create a block entry, all incoming email messages from that IP address are dropped at the edge of the service.
I suggest you refer the below document.
https://learn.microsoft.com/en-us/defender-office-365/tenant-allow-block-list-about