I think there's a bit of confusion in the Rails community about how and where to use the word "RESTful". Strictly speaking, the only thing that can be RESTful is your web API (as railsninja already mentioned). That the code of an application that conforms to the REST conventions (the application with REST API) can usually be organized into a set of controllers (that match the resources) and methods in these controllers (that match the four verbs of the HTTP protocol) is nothing but a hint of how to keep your application clean and organized.
If we want to talk about a RESTful Rails application, we can't just talk about RESTful controllers - there's nothing RESTful about just controllers themselves. It's possible to have a complex web application with only one controller (and myriad of methods) that represents many resources and is perfectly RESTful.
That said, it's pretty OK to add more methods to your controller. Sometimes, it's good to extract some of these extra methods and create a completely new controller - make this any time you feel good about it (rule of a thumb: create new controller anytime you are able to identify it with some self-sufficient resource, ie. a resource which could exist just by itself). Sometimes though, it'd be silly to extract some resource to a different controller. Say you have a resource which has a status attribute. It makes sense to perceive this status attribute as a resource by itself and perform at least one action on it (update), but it won't make any good to extract it to a different controller.