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Recently I was configuring Dynamics CRM client for Outlook on one of my machines in domain network. When I entered my server URL an error popped up stating:

“There is a problem communicating with the Microsoft Dynamics CRM server. The server might be unavailable. Try again later. If the problem persists, contact your system administrator.”

After some reading I figured it out that it might be because of any one of the following reasons mentioned below:

1> The OS system Date/Time/TimeZone on client computer is either not set correctly.

Make Sure that the client system is set to the correct Date/Time/TimeZone or is in sync with the Server Date/Time/TimeZone.

2> There are multiple bindings on the Microsoft Dynamics CRM website in IIS.

Open IIS, move to Sites and click Bindings in Action Pane on Microsoft Dynamics CRM website. Make sure that you have only one binding that is defined in the Deployment Manager.

3> Trying to configure RC(release candidate) version of Dynamics CRM client for Outlook against CRM server with Update Rollup 1.

We must have RTM version(05.00.9688.583 or later) of Microsoft Dynamics CRM client for Outlook installed instead of RC version (05.00.9688.53)
For the latest version of Microsoft Dynamics CRM 2011 client for MS-Office Outlook, Follow the below Link:

I checked for the 1st and 2nd option in my server, which looked quite OK to me. So, I uninstalled Outlook Client completely then downloaded the latest and installed it once again which solved my issue finally.

For further detailed Info on this, follow the Microsoft “Fast Publish” Article on this:
Article 1
Article 2
Article 3

Hope that would save a lot of Time while configuring CRM Client for Outlook.

Thanks !!!