On their profile card, tap the (⋯) located near the top-right corner.
On the bottom menu of the Xbox App, tap the (Chats).
Next to their gamertag, you should see a button labeled or a trash can icon. Tap it. A confirmation pop-up will appear asking, "Are you sure you want to unblock this player?" Confirm by tapping "Yes" or "Unblock" again.
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When their profile appears in search results, tap on it. If they are blocked, you might see limited information or a note indicating the block.