That depends on what you want to test, and how the app is written.
GUI is hard to test, but check out some of the other answers. If, as I suspect, you just want to test the business layer, that's easier:
If the app has the business and GUI decoupled, then you can easily use NUnit, either by integrating it into the project from your IDE, or in NUnit's own way, then write tests to cover what functionality the business layer exposes to the GUI.
If the app isn't decoupled, and you have a lot of the logic in the GUI, then you really need to refactor and decouple. Without doing this you will be restricted to testing via the GUI, which is difficult and not really full-proof, and it means trivial changes to the GUI may invalidate your testing of the business logic.