I use SmartClient and am quite happy with it and the support provided by Isomorphic. The U/I widgets aren't the nicest out there, but you can see that they've been around for some time by the richness of their API.
It's also quite easy to roll out your own custom controls when the built-in ones don't suit your needs. For example, we integrated Raphael pie chart SVG drawings inside custom Isomorphic canvas classes. We also integrated Mondrian/JPivot analytical technologies which are legacy JSP pages, using Smartclient's HtmlFlow control. It's quite powerful what can be achieved.
One thing I regret about Smartclient versus other technologies such as jQuery, is a clearer separation between the work a web designer does versus the work a developer/programmer does.
With Smartclient, it's mostly done thru code, even the layout of components. There's no HTML per say. They've separated very well the skinning (css), but that's about it. Everything else needs to be done by a developer/programmer thru Javascript code. Smartclient is good for single-page apps.
I can't speak for ExtJS as I haven't used it real production environments, but in the end I think it all boils down to the licensing model and programing/design model you want to be using.