A new organic-inorganic hybrid compound, H(C 5 N 5 H 5) 2 (C 5 N 5 H 6) 2 [Al(OH 6)Mo 6 O 18 ]⋅10H 2 O, has been synthesized and structurally characterized by single crystal X-ray diffraction, elemental analyses, IR, UV-Vis spectra and thermogravimetric analyses. This compound crystallized in the triclinic system, space group P-1, with a = 8⋅033(5) Å, b = 9⋅960(4) Å, c = 16⋅797(7) Å, α = 73⋅43(3)°, β = 87⋅85(1)°, γ = 81⋅47(1)° and Z = 1. The crystal structure can be described by infinite polyanions [Al(OH) 6 Mo 6 O 18 ] 3organized in layers parallel to the c-direction alternating with organic cations associated in ribbons spreading along the b-direction. Multiple hydrogen bonds originating from amine, hydroxyl groups and water molecules connect different components of the lattice.