Is it possible to use Razor on an existing ASP.NET 4 website?
marcind is correct, if you want to open your existing ASP.NET website in WebMatrix and work on it from within the tool. If, on the other hand (or in addition to), you want to use Razor syntax in your site and stay within VisualStudio, check out this article: http://weblogs.asp.net/rashid/archive/2010/07/10/use-razor-as-asp-net-mvc-viewengine.aspx
There are four things you need to do:
Add References to the Razor assemblies installed with WebMatrix. These can be found at C:\Program Files\Microsoft ASP.NET\ASP.NET Web Pages\v1.0\Assemblies
Create a custom ViewEngine class, a View class that inherits from IView (not that hard, check out the source in the article above)
Add your new ViewEngine in Global.asax Application_Start()
ViewEngines.Engines.Add(new RazorViewEngine(("cs"));
Create your view pages with a .cshtml extension, instead of .aspx
There are a few steps here, but it's quick work, and the source from the article above will get you a long way there.