Create an external tool in Visual Studio as shown below
Command : C:\Program Files (x86)\Microsoft Moles\bin\moles.runner.exe
Arguments: $(BinDir)/$(TargetName).dll /runner:"c:\Development Tools\NUnit 2.5.2\bin\net-2.0\nunit-console.exe" /x86
Initialize Directory : $(ProjectDir)
Now you can use Moles from within Visual Studio. :)