Never mind - I finally figured it out!

Adding the answer here just in case someone else sees this and has the same question :)

This is from member @Julia.LiMarzi from her post on this topic:

Manually suppressing a profile in Klaviyo is pretty simple. To manually unsubscribe someone from all emails sent by Klaviyo, navigate to Profiles > Suppressed Profiles > Add Email Address. Enter the email address and select Add Email Address. 

This method is what we’d recommend for suppressing a single profile at a time if, for example, a customer requested that you remove them from your list. If you are looking for more information on how to suppress multiple profiles at once for list cleaning, check out our article on how to identify and suppress unengaged profiles.

Unsubscribing and suppressing a user are two different things.  To answer your question the proper way to unsubscribe a user is search the user’s email address in the profiles tab > click on the email address > under “details” where it says “Email or SMS ” with a green check mark right click the 3 dots > select unsubscribe.  Suppression simply exclude the user from being sent marketing and should not be confused with consent.  Unsubscribe changes the consent value to not opted in.  For example, you may want to suppress a user that you know to commit fraud, but, you want unsubscribe a user that simply does not want your emails right now.