Visual C++ and Visual C# are not languages nor GUI frameworks; they are Integrated Development Environments - IDEs. This means they are text editors tailored to the task of development.
Visual C++ lets you code in C++, Visual C# lets you code in C#. Also, both let you create GUIs in a point-and-click manner.
Sounds like what you really want to do is create GUIs. In that case, without having further information, I recommend you go for C#. It is a much cleaner language than C++, it has fewer ways to shoot yourself in the foot, and it provides access to the immensely useful .NET framework.
C# features that C++ doesn't have:
Fully automatic memory management
Lambda functions¹
Type inference¹
Reflection
Remoting
Automatic serialization
True entity types
Properties
Database integration via LINQ
Convenient functional-style programming via LINQ
No header files
No undefined behavior
Direct interoperability with many languages
Compile once, run everywhere
¹ these features have been added to C++ in the C++11 standard.
C++ features that C# doesn't have
Template metaprogramming
Typedefs
Zero-overhead principle
Means to enforce const-correctness
Mature compilers that produce extremely optimized code nowadays
Much wider platform support