My experience is very similar to Laidoffsick.
To summarize:
Sculptamold - quick, neat, and easy to mix in small batches. Sets quickly (minutes) making it ideal for setting rock castings, filling odd gaps, etc. Downside - higher cost and not as strong as Structolite for a given thickness.
Structolite - very inexpensive (about 25 cents/lb). Very long setting time (hours) - mix a big batch and work all evening. Extremely strong - makes a good solid hardshell for scenery when applied in sufficient thickness (about 1/4 - 1/2"). Has a nice rock-like texture.
In the photo below, the horizontal layers directly behind the engine are Sculptamold. Sculptamold was also used to set the two large rock castings higher up the cliff and then covered with Structolite. Much of the rest of the cliff surfaces are Structolite.
When using different materials like this, it is important to prime everything with a coat of flat latex house paint. I used tan in this scene. Otherwise, the different surfaces will absorb color washes differently making it difficult to blend it all together.
Jim