Check out the MSDN developer center on WCF - it gives you a great intro and lots of reference material for WCF.
Basically, what you need to do is create a service contract - an interface that defines your service and its methods. Unless you only work with strings and ints, you will most likely also have to define a data contract - structured classes that will hold your objects going back and forth.
You then need a service implementation in a class that implements that service interface. This class will then be hosted inside your NT Service by means of a ServiceHost
(a class from the WCF runtime).
Typically you will define the "endpoints" (the URL's to call into and the protocols to use to do so) in configuration for your service - in this case, in your NT service's app.config
.
Once that's all up and running, your outside clients should be able to call into your WCF service running inside a NT Service.
Marc