Mike,
If you go look for a "Joel Bragdon's geodesic scenery" DVD, it will show you how to get the land forms you want using foam. His foam is just about like the Smooth-On you tried, but doesn't have the expansion. For land forms, if I remember right, you place the mixed foam on a piece of plastic (saran wrap) and then add a second piece on top and roll it out to a thin layer. Then just before really kicks pull one side off and drape over your land forms.
Maybe do a youtube search on it.