Hello Sean and Jeff,
This is a known problem caused by changes in the release version of .NET Framework 4. You can read more about the problem in the TestComplete FAQ:
My .NET applications are not recognized as Open Applications. Why?Complete support for .NET Framework 4.0 applications will appear in TestComplete 8.
There is a fix for TestComplete 7.52 that makes this version work correctly with applications created for .NET Framework 4 Beta 2 and earlier. Please contact our Support Team to get the fix:
http://smartbear.com/support/message/?prod=TestComplete