@olds-mike
I noticed two things I have no knowledge of...
He was using the PFS on sys:
and he was using two scsi controllers (scsi.device and warpscsi.device
If he's able to install the OS and run applications (I see Dopus and other things in his pics and vid) I'm assuming file system isn't an issue. I'd make sure you're installing
the latest version of PFS3-AIO from Aminet along with the C: (or at least PFSformat) tools from
the 53 install.
I was pretty intimidated by PFS the first time I used it, as well, and found the lack of documentation daunting. But it's a good FS especially for "more advanced" Amiga's (i.e., I'd use FFS if if I was just building something to play games).
Will try to load mine up later and post a few screenshots of the settings that work for me (disclaimer: your mileage may vary).

Two controllers shouldn't be an issue, but same as we've already talked about, may be simpler to eliminate as many possible causes of issues here as possible. Try them both on warpscsi.device. Hummm, I wonder if maybe there is some MaxTransfer or Mask issue... it validates the CD based on the video files on there, maybe it's having a problem reading those big files off it because those settings are off?
Post a screenshot of your CD0: device settings (the text file)?