I use Last.FM as a logging system for my music, nothing more. When I played music in iTunes there were no issues. But I use Pandora at my desk quite a bit, and I wasn't crazy about the work-arounds to get Pandora to work with Last.FM. There were various web-solutions that put a 'wrapper' around Pandora and logged the activity. The issue was a personal one, I don't leave my browser open and was often quitting the service inadvertently.
Enter Musicality. It is still a 'wrapper' in that the browser-version of Pandora is inside the shell of Musicality. But Musicality is not in the browser. It sits in my menu-bar and is a desktop based software. This allows some iTunes-like features, such as creating keyboard shortcuts to Like or Dislike a song. It works great with AirPlay as well.
So the only gap I have in terms of logging music now is Pandora on my iOS devices. Getting there.