Pi-hole works fine but unbound has a problem

Inquire if your ISP applies CGNAT for its customers?
I believe CGNAT doesnt work well with recursive resolvers like Unbound:

Some users were able to opt out of this CGNAT after contacting their ISP:

EDIT: When run below one, do you see an IP starting with 100.x.x.x which confirms CGNAT being applied?

traceroute -n 8.8.8.8

From the wiki:

The allocated address block is 100.64.0.0/10, i.e. IP addresses from 100.64.0.0 to 100.127.255.255.