I'd agree that it looks like there's something either in your application or the environment that the profiler doesn't like.
The first suggestion would be to ensure you've tried all the troubleshooting steps relevant to IIS and crashes in general as these help in a lot of cases. You'll find those links here
Often these things come down to a simple permissions problem.
If none of that helps, (or if the attach to process option works but not line/method level) it's likely that some component of your application doesn't like the instrumenting profiling methods. Sometimes we can work around these, sometimes not... post back if you're still stuck and we can get in touch directly to help out further.