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Hi Christina,
From what you've shared, it sounds like you've already covered several of the common troubleshooting steps. The account was working previously, webmail is still accessible, the account works on another PC, and you've already updated Outlook, restarted the Mac, and cleared the ADAL cache. Here are a few things you could consider trying next:
1/ Switch between New Outlook and Legacy Outlook
- If you're using New Outlook, try switching to Legacy Outlook and adding the account again (turn off the Legacy Outlook switch).
- If you're already using Legacy Outlook, try New Outlook instead (Help > Revert to Legacy Outlook.).
For reference: Outlook for Mac
2/ Create a new Outlook profile
- From Finder, open the Applications folder.
- Ctrl+click or right-click Microsoft Outlook, and then select Show Package Contents.
- Open Contents > SharedSupport, and then launch Outlook Profile Manager.
- Select the Create a new profile button, and then enter a name for the new profile.
For reference: Manage profiles or identities in Outlook for Mac.
3/ Test from a new macOS user profile
- Create a temporary local macOS user account and try adding the NHS account there.
- If it works, that would indicate the issue is likely specific to the original macOS user profile.
4/ Check with your IT team
It may be helpful to ask them whether there have been any recent changes to authentication, federation, Conditional Access policies, or Autodiscover configuration that could affect Outlook for Mac.
If needed, they can also raise a support ticket with Microsoft in casse the situation requires additional diagnostics or backend investigation.
If you are unsure who your IT admin is, you can refer to this official Microsoft guide for assistance: How do I find my Microsoft 365 admin? - Microsoft Support.
I hope your issue gets resolved soon. Any updates would be greatly appreciated.