I had a Kafka like problem today. I clicked the manage Organisation button in outlook,
File -> CRM -> Manage Organisations
The problem then appears saying
Microsoft Dynamics CRM for Outlook cannot be configured while Microsoft Outlook is running. Close Outlook and try again.
These seemed crazy, the manage organisations button is in outlook but you can’t run it whilst outlook is open.
This had me stumped for quite a while. I then remember that there is a diagnostic and configuration wizard installed.
Programs -> Microsoft dynamics CRM 2011 -> Configuration Wizard
Then from here you can edit or delete a CRM organisation from your Outlook