I cannot assign any users an issue other than myself (an admin) and the other admin on the site. Why is this? My users are granted access, assigned to proper groups, and given the proper permissions. But I can't assign them any issues.
You're now missing "browse" permission now. Note that if you grant "assignee" the "browse" permission, JIRA reads that as "anyone who *might* be assigned an issue", so that may not be much good to you. I'd also take a close look at all the permissions, as it seems someone has modified your scheme away from the (moderately sane as a starting point) Atlassian defaults.
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