iPhone, Android, and modern web browsers such as Firefox, Opera, Safari, Chrome, have excellent Javascript implementations, splendid CSS, and reasonable subsets of HTML5 -- but you can't use either fact if you also want to support Internet Explorer or other old browsers. Fortunately, Javascript frameworks such as jQuery and dojo can compensate in good part for such issues (I personally prefer dojo
, but jquery
's more popular, and the choice between two such good frameworks is more of a matter of taste -- plus, there are advantages with going for the popular choice, such as, you can probably get better support on SO;-).
For REST returning JSON, just about any decent server-side arrangement will be fine, so, you may as well stick with what you know best, in your case ASP.NET MVC (just as I'd stick with Python and Werkzeug on App Engine, and people with other server-side preferences would stick with theirs -- ain't gonna matter much;-). Client-side, pick one of the two most popular frameworks, Jquery and Dojo, and go with it -- both have good books if that's your favorite style of study, but also good online resources. (Less-popular frameworks surely have a lot going for them as well, but there are risks in getting far away from popular choices;-).
As a general/philosophical approach, Thin Server Architecture is well worth a look (except for one detail: they used to recommend XML rather than JSON -- dunno if they've seen the light since, but JSON's clearly the right approach so ignore any suggestion to the contrary;-).