In general it is a bad idea to make an entire terrain project out of these materials, but they can really help you get exactly what you want. The obvious idea is that you use them to make your terrain project look the exact way you want. The reason not to use them for the entire project is that they're rarely sturdy enough nor economical enough.
Sculpting materials that I've seen used a lot are:
I won't include foam for the same reasons I won't include wood or metal. People who use blue or pink foam a lot insist it is a sculpting material. It isn't. You can sculpt them by taking parts of the substance away, not by shifting its mass into a different shape. Besides I've already covered them in an earlier blog post.
Green stuff and Brown stuff are both forms of Kneadatite sculpting materials usually used by miniatures modelers. Some people because they're familiar with it use it on a large scale for terrain projects as well. This stuff is expensive though, don't waste it like that! Also, these materials are designed for being very finely sculptable... not for supporting heavy weights. Your finely sculpted terrain project may deform when heavy weight is placed upon it. But if you want to do something small with a lot of detail, like sculpt a miniature flower for the terrain scene you could use this just like you would with sculpting miniatures.
Brown stuff is very similar to green stuff with slightly different properties. Advanced sculptors use it in conjunction with green stuff when sculpting models. Most importantly all forms of Kneadatite are mildly toxic! Always wash your hands before touching your eyes, eating, or handling babies.
Clays and polymer clays. The big difference is that clays harden by drying out and polymer clays are designed to harden by baking. How much time do you need to complete your sculpting project? While these are used a fair amount, I recommend only using them on a limited basis because when they harden they also shrink and deform small amounts. On the plus side they can be fairly cheap (especially compared to green stuff!) and are very sturdy for storing or playing on.
Easily my favorite and most recommended is paper mache or Papier Mache for my french speaking wife. Basically made from paper and glue. It is cheap, sturdy, and doesn't deform while it hardens. The trick is not letting it deform while it is still wet! But you can add a lot of things to paper mache to make it harder initially. The same things you add to your mache can also be used to change the texture. Right now I've been experimenting with adding different kinds of sand to the mix because they give a different texture. Once dry it takes paint readily, after all it is made from paper and glue right?
Here is an example of how you can use it and the size of projects that can be made from it:
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