We could follow the steps below to remove the hybrid configuration from Exchange server. Please note that, it's recommended that you open a ticket and remove all vestiges under the guidance of a professional, as any accidental deletion would cause Exchange server to crash.
- Remove the organizational relationship from the on-premises environment
- Remove the organizational relationship from the Office 365 tenant
- Remove the federated domain(s) from the on-premises environment
- Remove the Email Address Policy/Policies associated with SMTP domains that have been moved to Office 365
- Remove the Accepted Domain entries from the on-premises Exchange admin console for SMTP domains that have been moved to Office 365
- Remove the federation trust from the on-premises Exchange environment
- Remove the remote domain associated with the Exchange hybrid configuration using the on-premises Exchange Admin Console
- Remove the SMTP send connector from the on-premises environment
- Remove the inbound and outbound SMTP connectors that were created by the hybrid configuration wizard
- Remove the HybridConfiguration object from within Active Directory
Detailed information can be checked here: How to Remove Hybrid Configuration From Exchange Server 2010
Please Note: Since the web site is not hosted by Microsoft, the link may change without notice. Microsoft does not guarantee the accuracy of this information.
Here is the a related thread discussed about the similar issue like yours: Roll back Hybrid Exchange to On-Premise Exchange
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