I originally started this project because I saw that web services were needed to interface DotNetNuke with ASP.NET AJAX. I think Creating Secure DotNetNuke ASP.NET AJAX Web Services is essential for creating secure DotNetNuke AJAX web services.
Now I am concentrating on Silverlight (see: A 3D DotNetNuke Dream). While Silverlight 1.1 allows for code behind interaction with DotNetNuke, for fast communication with DotNetNuke (for example to pull a piece of data from the DotNetNuke database) web services are again the best option.