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When you send an email from a CRM record in HubSpot, your picklist of “from” addresses pulls from two places: the accounts you’ve connected to HubSpot (and their verified aliases), and a list of aliases you manually added via the “Profile and Preferences” page in Settings.
Starting on February 25, all emails must be sent from connected accounts and their verified aliases; you'll no longer be able to send to manually-added aliases from within your CRM.
Moving forward, if you’d like to add a verified email alias to HubSpot, either connect that Gmail account directly, or add the alias to your Gmail account, and connect your Gmail account to HubSpot; any aliases you have set up for that account will be added to HubSpot automatically.