Seashells look prettier (boil first!), but yes, adding calcium to your tank will help your crayfish grow a healthier shell. Same thing goes for shrimp, crabs and other inverts with shells (snails, clams, etc.).
The shell/bone (well, since it's from a cuttlefish, cuttlebone really is more of a "shell" than a bone) will raise your ph/water hardness, so check your fish's compatibility for hard water. I would think in the overwhelming majority of cases the slight raise in ph/hardness would cause no effect on tankmates.