Are there any good GUIs that support Pygame surfaces as a widget within the application?
If this isn't possible or practical, what GUI toolkit has the best graphics component? I'm looking to keep the speedy rendering made possible by a SDL wrapper.
Dont use wxPython, its very hard to get to work well with Pygame, as described over at the GUI section of the Pygame wiki.
First of all, pygame relies on the SDL, which means that it can only have one window at a time. Thus, trying to implement multiple Gtk, Qt, ... application instances that use pygame, is an impossibility. The second problematic reason is that those toolkits use their own main loop, which possibly forces you to pipe their events to your pygame instance and vice versa. And to mention some other points in short: Drawing the toolkit elements on the pygame window is impossible and the SDL/pygame fullscreen mode will be problematic.
Instead, opt for any of the libraries listed at the bottom of that page. I use pgu myself.