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I took Udacity's cs101 class as a (lazy) way to get introduced to python. While I felt like it was a very well done introduction to computer science, it wasn't a very effective way to learn a language as it made a deliberate effort to decouple python and cs (and rightfully so). I would suspect that this is also true of the other MOOCs listed here.
Try MIT one, i guess that you will like. I have just started learning python ( after learning javascript ) in i find it best resource available.
Also, Project Euler for "Practice Exercises and Projects", and vim+python-mode and geany for IDE's.

python-forum.org and #python on irc.freenode.org for getting specific help.

Python as a language is great. Its the GUI frameworks that always stop my advances into Python...there are about half a dozen of them and they come in various flavours of broke, ugly, incompatible, difficult or abandoned.

So I end up downloading VS C# Express...

As someone who's relatively comfortable with VS ('08-'12) and who has licenses, I'm curious to know what the limitations (if any) are to using VS for development with Python.

Do you (or does anyone) know of any quick-start guides or tutorials to working with Python (or any other non-.NET languages) in Visual Studio?

All the code on the internet is C#, so I don't really both with python on VS. I guess its possible, but for learning it strikes me as a bad starting point.
I haven't used it much with Python, but I had a great experience with Qt with C++ and I know Python bindings exist. How much have you looked into it?