Default LAN settings work for everything except Unraid Connect and checking for updates on anything; my shares are all accessible and my containers are running without issues, and the only thing changed right now is removing the bond to allow the full speed of the connection I'm using.
Configuring DNS manually to OpenDNS did cause the entire thing to lose connection though, as at that point it failed to grab an IP after rebooting (still attempted to get DHCP, but it didn't set; this is the only device on my network which does this, my main Windows machines and Linux machine have all survived manual DNS and still grabbed IP from DHCP). I'll try a sanity check with a different router (non-firewall) when I have a day off, as after my 12 hour shifts I just want to stop and chill until I pass out; give me a few days to finish out the week and I'll mess with my network on the weekend and report back.
As an additional note, in case it helps, it has run on two different PFsense setups in the time this issue has been happening, and it occurred on both. The only thing configured on either PFsense is DHCP, which sets the IP range to 10.0.0.x/8 and DNS to 10.0.0.2, which is a container on the Unraid server (again, same on both; configs only have that changed from default).