Yes you can create applications targeting .NET using VC++. You need to use the /clr flag to tell the compiler that you are targeting the CLR (common language runtime). There are additional options available for /clr so check out Microsoft's info about it. In most cases /clr without options will be sufficient.
Unless you have a specific need to mix native code (= unmanaged C++) and CLR byte code (= managed C++) I would recommend using a language that was designed specifically for .NET. C# is the prime candidate. With a good C++ background you will find that C# as such is not the big challenge. You probably will spend more time on learning the class libraries.
Regardless of the language you use to produce byte code for the CLR, the .NET framework needs to be available on the target computer or device. Microsoft provides that either as part of the operating system or as a separate download. As an alternative, in particular for non-Microsoft platforms the Mono project might be an option.