You can unassign users groups from a role collection by deleting them from the role collection.
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Open the SAP BTP cockpit.
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Go to your global account and subaccount (see Navigate in the Cockpit).
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Choose Security > Role Collections.
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Choose the role collection from which you want to unassign a user group.
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Go the to User Groups section and choose 🗑️ (Delete).
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Confirm the popup and save your changes.