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Oh, wow. So, what I had to do was format the oversized SD card(s) to FAT32 with my PC. I guess I did that back in 2015, then completely forgot about it over the last 3 years. I couldn't even remember what program I used to do it (since Win7's default program won't do it), so I had to use something else I downloaded last month for upgrading the storage on my Nvidia Shield.
http://www.ridgecrop.demon.co.uk/guiformat.htm (used a 64k allocation, assuming that will improve performance)
@Fade2black001 , I gave you some wrong advice in this thread: https://gamefaqs.gamespot.com/boards/918340-playstation-portable/76791226
Everything after the second quote in #7 is incorrect. I'm very sorry about that, my memory played tricks on me and I was confused about a few things. See above. Sounds like you may have already known formatting a card to FAT32 was all that was required for a single-card adapter, so hopefully you figured it all out for yourself. Also, most of the problems I mentioned with memory cards >64GB, in my case, were actually caused by a faulty UMD drive which was causing the Home Screen to stall everytime it tried to load. I "fixed" that for now by putting enough duct tape over the lip of the UMD drive lid that it never fully closes. With the UMD drive open and effectively disabled, I now only experience the normal, very minor, slowdown associated with >64GB cards.
Again, sorry to everyone here for posting misinformation in that earlier thread, it was an honest mistake.
UPDATE: To make the 64GB+32GB dual adapter work, I had to format it first with GUIFormat (which gave me a 64GB card), then again with my PSP (which gave me the full 96GB). No idea why that worked when so much else didn't, sigh. If I was writing the retro-ownership FAQ this system begs for, I would research/experiment with this mystery until I understood it inside and out, but for now, I'm just glad my problem is solved...