So I have a group of users that I want to prevent from being assigned to specific projects. Is there a way to do that other than removing them from an all-purpose group that most users are already in?
No, permissions in JIRA are inclusive. To exclude them, you have to remove them from the roles/groups/whatever that you have used in the permission scheme to say "they can be assigned issues"
Hello Lee,
In additional to Nic's response, I'd advice you to take a look here to have more information about how to manage JIRA projects permissions.
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