From the RetroPie-Setup I uninstalled unnecessary components -- remove WolfRam, SonicPi, etc. Nothing more than a boot to emulator, so I figured I would get some clutter out of the way.
I then went back to trying to different gamepad configurations through the driver config file. I enabled all four ports and through sheer dumb luck GPIO7 (gamepad4) started reading. I still cannot get GPIO2 / GPIO3 to read the data from the controller, but I have two working NES controllers right now!
I also tweaked the /opt/retroarch/configs/all/retroarch.cfg
There is a setting for joypad input scan cycle -- something along those lines -- that I opted to put at a value of 0 (I am trying to recall this from memory as the NES is now wrapped under the tree for dad) so that it would update controller state on demand. It was defaulted to 2 and the notes in the file were about adjustments for latency issues.
I also had to copy the configuration for player1_input* and update it for player2 within /opt/retroarch/configs/all/retroarch.cfg.
Also removed the override line from /opt/retroarch/configs/nes/retroarch.cfg
Still no idea why I cannot access GPIO3 / GPIO2 -- if anyone has any troubleshooting ideas I would be happy to jump through the hoops. I have the other SD card and another Pi3 at home I can run through.