If you are already familiar with html, you might consider using the browser for the UI. It's pretty much cross-platform, if you ever need that, and users are accustomed to browser look/feel.
If your installation doesn't already have a python-enabled http server running, there are several options (python CGI scripts, cherrypy, kerrigell), any one of which is easier to learn and more generally-applicable (I think) than any of the gui toolkits. Ron -- http://mail.python.org/mailman/listinfo/python-list