[CN3H6](2)[Zn(CO3)(2)], the first organically templated open-framework carb
onate has been synthesized hydrothermally and its single crystal structure
and some properties have been determined. This phase is built up from a thr
ee-dimensional framework of vertex-linked ZnO4 and CO3 building units encap
sulating the extra-framework guanidinium cations. Template-to-framework hyd
rogen bonding appears to play an important role in stabilizing the structur
e. The zincocarbonate framework shows a surprising similarity to those of k
nown zinc phosphates and phosphites.