It depends on how you define "Best." There are various elements that need to be supported by a modular test structure, and the choice is mainly friendly to the developers. I have used NUnit / MSTest in the past, and I like NUnit because it not only supports various mocking structures like NMock, RhinoMock, MoQ, etc. it also makes life easier when you can directly run unit tests from the NUnit user interface without opening the VS interface.
If you are using VS2008, then you can also use MSTest or NUnit ....
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