Can I group devices based on interface alias?

there’s a way to use instance level properties like the aforementioned interface aliases to help group devices as well?

There’s always a way; multiple usually. The way I’d start would be to create a custom propertysource that grabs the instances for the device from the LM API and stores a device level property containing a list of the service provider names (not a trivial thing, but not the hardest in the world). That way you’d have a property you could use to group the devices based on whether that property contains “Comcast” or “Sprint” or “ATT” or whatever.