You can delete memberships of user accounts in system entitlements.
To delete memberships
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In the menu bar, click Data > Data Explorer.
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In the Data Explorer navigation, click System entitlements.
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In the list, click the system entitlement with membership that you want to delete.
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In the details pane, click the Memberships tab.
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On the Memberships tab, click Directly assigned.
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Select the check box next to the membership you want to delete.
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Click Delete.