Seems like it would be a good way to introduce some people to unit testing.
Well for one thing, the documentation for doctest talks about "interactive Python sessions". There's no equivalent of that in C#... so how would the output be represented? How would you perform all the necessary setup?
I dare say such a thing would be possible, but personally I think that at least for C#, it's clearer to have unit tests as unit tests, where you have all the benefits of the fact that you're writing code rather than comments. The code can be checked for syntactic correctness at compile-time, you have IntelliSense, syntax highlighting, debugger support etc.
If you're writing code, why not represent that as code? Admittedly it's reasonably common to include sample code in XML documentation, but that's rarely in the form of tests - and without an equivalent of an "interactive session" it would require an artificial construct to represent the output in a testable form.
I'm not saying this is a bad feature in Python - just that it's one which I don't believe maps over to C# particularly well. Languages have their own styles, and not every feature in language X will make sense in language Y.