The only fully portable GUI for Python is the standard TkInter, if you don't want any additional install beside Python. The Python's 3.1 Themed Tk is quite nice looking, compared to the older Tk version.
A few weeks ago, I had to answer the same question as you. I came to the conclusion that PyQt is currently the best choice for a modern, powerful, well-maintained, and portable GUI, mainly because of some of the shortcomings of its main contender (wxPython, see below). (Tk, and Themed Tk would be good for simpler needs.)
Two words of warning against wxPython: it is not possible to install it via the popular Fink package manager on Mac OS X, currently, which makes it far less portable than PyQt and TkInter; it is also not yet Python 3-compatible, as far as I know.