Hi
Sync is only possible from On-Premises to Azure AD, it can't happen the other way. If you need to create on-premises identities for Cloud users, run an export using PowerShell or GraphAPI and use the attributes to create the users on-premises. Once you set our Sync up, you can use "soft-matching" to match the identities and passwords:
Question on this - you say there is no sync in place at present, do some users have accounts both on-premise and cloud? If so, you can just soft-match these once sync is set up.
Hope this helps,
Thanks
Michael Durkan
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