During the reaction CaC4O4 · 2.5H2OCaC4O4 · 1H2O + 1.5H2O single crystals remain undisturbed and lattice dimensions practically identical both in the water-rich and in the partially dehydrated form. In both hydrates Ca2+ and C4O42− build up a three-dimensional framework with open channels. The zeolitic character of part of the water results in a random occupation of lattice sites.