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You can absolutely add contacts to the unsubscribe list manually. There are a couple methods that you could use depending on the amount of address that you are trying to unsubscribe at a time. Click Here for instructions on manually unsubscribing one contact at a time.
Next, you can also upload a spreadsheet of email addresses that you intend on unsubscribing. In order to do so you would have to enable the advanced contact permission settings. Click Here for instructions on doing so. Once these advanced permissions have been activated you can upload your list of unsubscribes. Click Here for those instructions.
I sure do hope that this helps! Thanks again for your post, have a great weekend!
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