More info on this:
I was having trouble with the web.config issues as well and remedied that by ensuring web.config was not open in the code editor when I dragged and dropped the Chart control onto the page. If web.config was not already open, Visual Studio 2010 would make the appropriate modifications.
I was able to successfully get past the "error executing child request" error after successfully applying the web.config issues.
Also regarding usage in an MVC application, I was struggling to implement this in my MVC 2 application (VS2010/.NET 4) and ran into another gotcha.
The page's call to ChartImg.axd was resulting in an HTTP 404 error. (I found this using Fiddler.)
It turns out the page was trying to access the handler from /MyController/ChartImg.axd instead of /ChartImg.axd (from the root).
I was able to fix the problem by adding this line to my Global.asax.cs file:
routes.IgnoreRoute("{controller}/{resource}.axd/{*pathInfo}");
This might have been the problem for some users who had to resort to changing the Chart.ImageStorageMode property.