@coltonu
That is almost the same thing in klaviyo, even when people unsubscribe themselves they are suppressed (just the reason for suppression is different and says unsubscribe instead of manual suppression for those that you manually suppress) but there is no option for you to do this manually and to say that they unsubscribed on their own.
From what you are asking the only thing i can suggest is maybe deleting them instead of suppressing them, this way they will be removed from the account fully (but this way you are losing all data you have about them)
In this article you can find more info about any of these things.. https://help.klaviyo.com/hc/en-us/articles/24312135764251
I 2nd @Bobi N. klaviyo mark them as suppressed if soemone unsubscribe.Btw why you want to unsubscribe them means what you want to do