@Mcat12, thanks for the help.
I'm not sure how I missed it previously, but this appeared in tonight's frantic searching:
After trying a bunch of stuff, it was that edit to /etc/NetworkManager/NetworkManager.conf
that got everything running again.
On my initial install of pi-hole, I had to remove /etc/dnsmasq.d/network-manager
...maybe some recent Ubuntu Mate package updates decided to change up the Network Manager settings again.
I'll certainly think twice before my next apt-get upgrade
...