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The title compound, {[Ni(C2N3)2(H2O)2]·2C5H5NO}n, is a centrosymmetric two-dimensional coordination polymer with a layer (4,4) network structure. The asymmetric unit is compossed of an NiII atom, which sits on an inversion center, a μ-1,5-bridging dicyanamide anion, a water molecule, and a free 4-hydroxypyridine molecule present in the zwitterionic pyridinium-4-olate form. The NiII atom is coordinated in a slightly distorted N4O2 octahedral geometry by four bridging dicyanamide ligands and two trans water molecules. In the crystal, the two-dimensional networks are linked via N—H...O and O—H...O hydrogen bonds, forming a three-dimensional network.