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I'm trying to create a memory card, and an error message stating "The Operating System prevents this file from being created" pops up.  My OS is Windows 10.  Is there a way around this, or is it not doable?

Make sure you're running PCSX2 as admin so that you have proper read/write access to the folders.

Alternatively you can also place PCSX2 in a folder that isn't My Documents or Program Files. (C:\PCSX2 instead for example)