I've used GTK and Qt in C++ and also PyGTK and PyQt in Python quite extensively.
Qt beats GTK hands down - its a much more flexible, modern and clean API. GTK is also lacking some features that are important to me. From a framework point of view, I'd recommend Qt.
As for langauge bindings (I can only speak about Python, since I've never used the Ruby equivalents), I think PyGTK (using Glade and a wrapper like Padraig Bradys libglade) make GUI programming insanely easy and fun. However, if you can GPL your software (or pay the license fee), then PyQt is also a good option, and while not quite as friendly as PyGTK + Glade (in that with GTK you can define your UI in Glade as a separate XML file, so you can tweak the UI without touching code; in Qt if you want to use QtDesigner, you have to generate code using uic, if I remember correctly) the API itself is really really nice to use and mirrors the Qt frameworks clean design very closely.
Over all, I'd probably recommend using PyQt over PyGTK, but I may be biased since I much prefer Qt over GTK nowadays, though you could try both out and see which you prefer - they are both almost trivial to get working.
If you are looking for a great book on PyQt, I'd recomment Rapid GUI Programming qith Python and Qt.
To summarize: IMHO Qt beats GTK in both quality and capability. Both PyGTK and PyQt are of excellent quality and capability mirrors the underlying framework, though PyGTK can load Glade xml files.