A very common approach to implementing RESTful services is by utilizing ASP.NET MVC to do so over WCF.
ASP.NET MVC has excellent RESTful support by via flexible URL rou
WCF services can be self-hosted. No IIS required. ASP.NET MVC is focused on delivering HTML, whereas the existing .net 4 WCF stack is focused more on XML and JSON.
The new http://wcf.codeplex.com is the next generation of REST on WCF and will be significantly more capable than the existing stack.
The new stack will be much better at supporting all different media types. It provides much better access to the underlying HTTP protocol. It will be much more testable and will make it easier to plug in reusable handlers to add standard behaviours.
Take a look at Podcast from Scott Hanselminutes with Glenn Block where they discuss same issue and compares MVC and new WCF Web API. http://www.hanselminutes.com/default.aspx?showID=284
I'd say WCF is better suited to build services, you can do it with asp.net mvc but it requires more ceremony