I'm not sure what programming languages your familiar with, but as far as gui programming I like to use the QT toolkit from trolltech. QT is the gui library that KDE uses. There are bindings for many languages but QT itself is a C++ entity.
GTK+ (which gnome uses) and Motif are other popular GUI toolkits.
I guess I'd recommend getting QT's dev package (if you don't have it already) and learn how to use designer and/or kdevelop.
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