Anything can work for making a mold, all depends on the skill of the maker and what type of jig you want to make. I have tried making basic ones out of USG plaster but never got them lined up for lead pouring and they failed miserably. I have been thinking about making one out of plaster or concrete that I need and doesn't have 2 sides to it. Kinda like a flat bottom plastic worm mold. Let us know if you try the hydraulic concrete, maybe it will work well.
I love taking my kids fishing, now if I could just manage to fish at the same time.