Should I Remove Built-in Administrators from the Operating System Permissions?

I really wouldn’t recommend doing that. Instead of removing them, it’s better to secure these accounts. You can refer to Microsoft's guidelines on securing built-in administrator accounts for best practices.

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Here’s a note from Microsoft: The 'Act as part of the operating system' permission is quite powerful, allowing users to take full control of a device. It’s advised to restrict this permission to as few accounts as possible. Typically, it shouldn’t even include the Administrators group. Instead, when a service needs this privilege, you should configure it to run under the Local System account, which already has the necessary rights. Removing those accounts shouldn’t have much impact since the 'Act as part of the operating system' is rarely needed by anything other than Local System.

Honestly, if it ain't broken, don't try to fix it. Trying to remove those accounts might end up breaking something critical.

There’s really no good reason to completely remove them. There are established frameworks suggesting safer alternatives instead.