You need to weigh several things..
If you are dealing with a low-traffic, internal web application, perhaps server-side postbacks are the way to go. Often you'll find that there's less code you'll have to write in this case.
If you are working on an external, public, high-traffic web application, perhaps AJAX is the way to go. That way you avoid posting back entire ViewState and running through the full page lifecycle. This may result in more front-end code, but is less load on the web server.
Keep in mind that client-side data binding is a very viable solution these days, with the help of such things as jQuery Templates. So that helps bind data returned from AJAX calls to tables and other elements.
As far as web services go, they are great for when you're sharing data/functionality between different systems. If you don't foresee doing that for this particular application, then perhaps there's no need to over-engineer it - keep it simple with either MVC and Action methods that support AJAX calls out of the box, or get familiar with PageMethods.
I'm sure there are other pros/cons I haven't mentioned, but this is the first thing that came to mind.