It is very easy to unsubscribe a contact manually. First visit the Contacts page and search for the contact that you wish to unsubscribe. Click on the name of the contact that you wish to unsubscribe. You will then need to click on "Permission to send" near the contact email address.
From this menu you will be able to manually unsubscribe this contact. Be sure to click "Save" to finalize the changes.
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