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What exactly do you mean by have Windows unload a .dll? Have you tried searching MSDN to find the Windows API functions that would unload a .dll in the desired manner? If you could find that in the Windows API you can call it in LabVIEW. Let us know what you find.
This only works for DLLs loaded in Labview, causing a 3rd Party Programm or windows itself to unload a DLL you will need do adress a function that will do this for you.
Can I Dynamically Load and Unload a DLL in LabVIEW?