Mike,
The Tkinter module, which is actually used to make GUIs appear on screen that you can interact with, comes with Python be default. You are after a GUI program to help you build/design Tkinter GUIs (I'll call it a GUI builder). For the most part these things let you lay out the GUI, hopefully from there it will look nice, and all you need to do is insert the magic behind the scenes to actually do the calculations when you click the right buttons.
However, in all honesty (and I have really tried to make them work), these kind of GUI builders are just not that great. They tend to hide a bit too much from you, so when you come to inserting the code that does the calculation, it is pretty unclear and difficult. That is if you can actually get the right bits in the right places, layouts, get it to do the right things if the window is expanded/shrunk, etc.
In my opinion, you are best off just to get a good textbook for the GUI module you wish to use and learn it the hard way; fortunately it is usually not that hard (I have done a bit of Tkinter, a reasonable amount of WX, and some Qt), and you will learn a huge amount about Python in the process! Once you actually know how the GUI environment works, then have a go with the GUI builders (i.e. you will know the real difference between a Grid Bag Sizer and a Box Sizer when selecting them from the menu).
Which language to use?
[INDENT]Tkinter is nice in that it comes with Python (no extra installs required), but that is its only positive - it looks like something from Windows 3.1, is definitely the most confusing to learn, and the online documentation is horrific (not sure if it hasn't been updated for the past three versions, or is just plain wrong). WX and Qt are fine - but of the two I would probably recommend Qt - it seems to be a bit newer, more cutting edge, and has some really good, accessible documentation.[/INDENT]
Let us know how you get on!