A good excercise would be trying to understand other people's C# code snippets, and reproducing them yourself from scratch. This means that you'll encounter lots of stuff you need to look up and learn in order to understand to see what those snippets are doing.
The good news is that, both in C# and VB.Net, the .NET framework does most of the heavy lifting, so you'll probably understand and recognize those parts. I use both C# and VB.Net in my job and I've come to realize that, because of the shared framework, the languages aren't that different from each other in practice.
I still like C# better, since I feel it results in cleaner code, somehow.