Figured I should leave this breadcrumb here in case I (or anyone else) brainfarts on this like I did.
I had also encountered the following problem
```
NVIDIA-SMI has failed because it couldn't communicate with the NVIDIA driver. Make sure that the latest NVIDIA driver is installed and running.:
```
and couldn't figure out why unchecking the vfio-pci binding didn't unbind my GPU.
Then I realized I had followed this guide on GPU passthroughs, so of course the VFIO drivers would remain bound.
I simply went back into Main > Flash > Syslinux configuration, and under [Unraid OS], changed from
```
kernel /bzimage
append video=efifb:off vfio-pci.ids=10de:1e89,10de:10f8,10de:1ad8,10de:1ad9 isolcpus=4-7,12-15 initrd=/bzroot
```
back to
```
kernel /bzimage
append initrd=/bzroot
```
After a reboot, the NVIDIA drivers did their thing, and my Docker containers are now using the GPU. 👍