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In the title compound, Na3(C6H15N5O)2[Al(OH)6Mo6O18]2Cl·20H2O, the [Al(OH)6Mo6O18]3− polyoxoanion has a B-type Anderson structure exhibiting approximate D3d symmetry. There are two types of sodium cations: the Na+ cations of type I have a distorted octahedral coordination geometry formed by six O atoms and are statistically distributed over two positions with equal occupancies, while the coordination polyhedra of the two Na+ cations of type II share one Cl anion located on an inversion center. The latter fragment, containing a Cl anion and two sodium cations, links two polyoxoanions into centrosymmetric blocks. The diprotonated 1-[imino(morpholino)methyl]guanidinium cations and uncordinated water molecules contribute to extensive N—H...O and O—H...O hydrogen bonding, resulting in the formation a three-dimensional supramolecular structure.