I've seen (tho never tried) two interesting techniques for both the structure and the finish.
Structure:
1 - polystyrene foam pieces, cut to resemble rocks and branches and whatever you want, glued to a board. Best for rocky walls and such.
2 - spray expanding foam, either on a board or directly in the enclosure. Place branches, hide and such on your base and spray all around. You can carve it to your liking once hardened.
Finish:
1 - a few layers of diluted tile cement on the foam, then water based paint to make it look like rock, wood etc.
2 - cover every piece of foam with a thick layer water based silicone, press some coco fiber substrate on it and let it dry. Remove the excess once dry.
Google is your friend for some pictures.
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