I think solving Top-Coder problems will be great practice! It's specially suited since all their problems are console based, and they will make you increase not only your knowledge of c#, but also your problem solving skills and your data structure/algorithms knowledge.
That said, you probably wont learn much about new or more platform specific stuff about C#, such as linq, event handlers, threading, parallel tasks library, etc etc. For that, the best would be to find a good C# book and go through it.
Another way could be making little games. I know its console, but you can actually make games like Snake, Pac-man, hangman, etc, of course, with a little extra imagination, but it still works and games are great learning exercises (and are fun to show to people)