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To learn the full process to import customers via CSV, read Import a list of customers via CSV. If you are importing a significant number of customers the best way to unsubscribe them is to upload a CSV via the Import/Export page. To do this create a CSV with the list of emails you want to unsubscribe in one column and in a second column with the header tags and the word unsubscribed in that column. 
email,tags
    chris@example.com,unsubscribed
    james@example.com,unsubscribed
    rory@example.com,unsubscribed
Once imported, all of the customers that have the tag ‘unsubscribed’ will be marked as unsubscribed.