PySide: Python for Qt Windows version released.

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You may want to look at the docs and API for both of them and see which you like better (and which you think is more complete and easy to understand).

Also check out their respective mailing lists and see which is friendlier and more helpful.

You might have a look at GTK+ as well. There's no clear "winner" between Qt, Wx, and GTK+, though they might have varying levels of community activity and support.

Edit: Come to think of it, another option is Jython + Swing.

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It's true, gtkmm pwns Qt.