Plaster of Paris is my go-to material.
I use Styrofoam as the base material to get the major shapes and land forms. If necessary to use more than one layer of Styrofaom, I'll hot glue the layers together which is much faster and water proof than using white glue (PVA).
I then trowel plaster on to that. As the plaster sets, you'll have about 15-20 minutes where it is soft and plastic, and this is my optimal time for the carving and scribing. So, I only work in an area that's not so big that I can't do all the scribing in that time. With practice, you can mix, trowel, and scribe repeated areas fairly quickly.
Here're a couple of examples of stone work and cobbles done with nothing but plaster over Styrofoam - all scratch built:




It's "old school," but effective and very flexible. You're never limited to a design or composition created by someone else.