CN3H6. Al(HPO4)(2). 2H(2)O, prepared by hydrothermal methods at 120 degrees C, contains infinite stacks of guanidinium cations (intermolecule C ... C separation similar to 3.5 Angstrom) interleaving a distinctive anionic aluminophosphate layer topology based on polyhedral eight-rings of vertex-sharing AlO4(OH2)(2) octahedra and HPO4 tetrahedra. Crystal data: CN3H6. Al(HPO4)(2). 2H(2)O, M-r = 315.05, orthorhombic, Pnma (No. 62), a = 6.965(2) Angstrom, b = 20.624(4) Angstrom, c = 7.168(2) Angstrom, V = 1029.7(5) Angstrom(3), Z = 4, R = 3.42%, R-w = 3.40% [85 parameters, 829 observed reflections with I > 3 sigma(I)].