To clean up tattooed Group Policy Preferences (GPP), create a temporary cleanup GPO and use the Delete action rather than attempting to enable “Remove this item when it is no longer applied” on the original GPO. Since the original GPO has already been unlinked, enabling this option retroactively will not remove the settings from affected systems.
The reason the settings persist is due to the tattooing behavior of Group Policy Preferences. Unlike traditional Group Policy settings, GPP writes values directly to locations such as the registry and does not automatically remove those changes when the GPO is unlinked or no longer applies. The “Remove this item when it is no longer applied” option only works when the preference item was originally configured with that setting and the GPO remains in scope long enough for the client to process the removal. If the GPO is removed first, the tracking mechanism is no longer available.
The cleanup process is to create a dedicated temporary GPO and target it to the affected computers or users. Within this cleanup GPO, configure a Registry preference under Computer Configuration or User Configuration > Preferences > Windows Settings > Registry and set the action to Delete for the specific registry key or value that needs to be removed.
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hth
Marcin