Layered zincophosphate materials were prepared from the molecular precursor Zn-4(mu(4)-O)[O2P((OBu)-Bu-t)(2)](6) (1) via thermolysis (180-215 degrees C) in anhydrous organic solvents in the presence of long-chain primary amines. Through variation of the amine concentration, two series of materials were obtained with the stoichiometries Zn-2(HPO4)(3)(H-3-NCnH2n+1)(2) and Zn-2(HPO4)(3)(H3NCnH2n+1)(2)(H2NCnH2n+1) (n = 8-16) These materials possess an unusual Zn/P ratio of 2:3 which is uncommon for layered zincophosphate materials prepared in aqueous media.