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I've been trying to use the Alert Policies in the Office 365 Security and Compliance center to build an alert policy for a single high security document library. I want to get an alert for when people outside of a certain group of users access any of the files within this document library, and only this document library.

However, I've only managed to limit the alert policy to site collection level, and not document library level. I don't want to get an alert for when people access files in the same site collection, but in a different document library. Is there a way to limit the scope of the alert policy to just that single document library? I have tried setting the alert policy to use "https://********.sharepoint.com/sites/YouthAndInternships/FormResponses*" as the Site Collection URL, but that just makes it so that the alert policy is not triggered at all.

The setup of the alert policy is here:

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I did a test on my end and got the same result as yours. Seems that the Minimum level of activity "Accessed File" is site collection level. It's impssible to limit the policy to document library level.

As a workaround, I would suggest you create individual site collection for this library.

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