Well, I couldn't possibly give a better answer than Dr.Deo, but I can share my bit. I used to do a lot of GUI programming before (more than 5 years ago, with Borland's VCL in either Delphi or C++). I recently had to produce a GUI for a little project, so I went for Qt4. I was able to almost entirely finish the GUI in one day without any prior knowledge of Qt4 (of course, it was a simple, one-window GUI). I found it very easy to use and quick to learn. If you have any GUI experience at all, it will be very intuitive. As for C++ knowledge required, it's minimal. You have to be comfortable with a fair dose of inheritance and polymorphism, but that is very typical of GUI tools and it really is just basic C++ knowledge of OOP.
I think several people have already made the point about being cross-platform. This will be more and more important in the future as alternatives to Windows are becoming mainstream (basically all the people I work with either have a Mac or run a distro of Linux) and as more in-between phone and tablet-PC products are emerging.
And, anyways, the language you use for programming a GUI isn't really that important, it is the tool-set. I think Qt4 is very complete. It also save you the trouble of interfacing to your existing code (let alone learning C#). Finally, Qt4 is very nicely usable with any IDE or build system (if you don't want to switch your code to qmake and/or Qt-Creator).