Click Use as System Photo Library greyed out so can't select to set new System Photos Library
"Click Use as System Photo Library" greyed out so I can't select to set new System Photos Library to access iCloud photos
MacBook Air
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To choose a new system library you need to open that library.
Quit Photos. Then option-click the Photos icon. You will get a list of your libraries and the option to create a new one.
When you've created or opened a library that's not your system library, "Use as System Library" won't be grayed out, and you can designate this new one as the one.