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The crystalline product (NH4)2[Zn(C3H7NO)(H2O)5]2[V10O28]·4H2O was successfully isolated from an H2O/DMF solvent combination by evaporation at ambient temperature. The salt crystallizes in the P21/n space group. Imidazole, initially used in the synthesis but not present in the product, and DMF solvent appear to affect the synthesis and crystallization as structural-directing agents. In the title compound, the complex cation [Zn(H2O)5(DMF)]2+ acts as a counter-ion without being directly coordinated to the decavanadate anion. An extensive framework of hydrogen bonds integrates the whole architecture as evidenced by X-ray crystallography. The polyoxometalate [V10O28]6– lies on a center of symmetry while the complex cation [Zn(H2O)5(DMF)]2+ links three adjacent anions through a set of 2 + 2 + 3 hydrogen bonds.