My account is is in the Administrators group; why can't I modify files under the "C:\Windows" directory?

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Because Administrators cannot automagically edit all files. Have a look at the file fle permissions, and grant the "Administrators" edit permisions.

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It depends what you want to modify.

Some files as Daniel said are protected and you will need to modify permissions, however, other files could actually be running/in a process and be locked from modification.

Please indicate the name of the file you are having problems with and I can try to help further.

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