I did follow the directions to the letter. What I did next was to edit the webconfig file to allow me to see the exact errors that were being encountered.
Turns out that the temp directory for .NET framework 4.0 did not have the proper permissions for the service account (Network Service). I had to run Microsoft's tool (ASPREG_IIS) to effectively modify access and "reset" the .NET framework.
Once I did this, I restarted the web service and everything started working.
Thanks for the rapid response! I hope my experience helps others who may run into this issue with .NET framework hiccups.