Thiosemicarbazide complexes of nickel(II) [Ni(TSC) 2 ](HSal) 2 (I) and copper (II) [Cu(TSC) 2 ](HSal) 2 (Ia) (TSC is thiosemicarbazide and HSal is a salycilate anion), as well as complexes [Ni(TSC) 2 ](SO 4 ) ⋅ 2H 2 O (II) and [Ni(TSC) 3 ]Cl 2 ⋅ H 2 O (III), are synthesized and characterized by IR spec troscopy and X ray diffraction. Monoclinic crystals I and Ia are isostructural; space group P2 1 /n, Z = 2. Crys tals II are monoclinic, space group P2 1 /m, Z = 2. Crystals III are orthorhombic, space group Pbca, Z = 8. In I and Ia, two planar salycilate anions sandwich a planar centrosymmetric [Ni(TSC) 2 ] 2+ cation to form a supermolecule. The cation and anions are additionally bound by hydrogen bonds. Other hydrogen bonds connect supermolecules into planar layers. In structure II, centrosymmetric [Ni(TSC) 2 ] 2+ cations are con nected by π stacking interactions into supramolecular ensembles of a specific type. The ensembles, water molecules, and (SO 4 ) 2-anions are bound in the crystal via hydrogen bonds. In the [Ni(TSC) 3 ] 2+ cation of structure III, ligands coordinate the Ni atom by the bidentate chelate pattern with the formation of five membered metallocycles. These metallocycles have an envelope conformation unlike those in I and II, which are planar. In III (unlike in analogous complexes), a meridional isomer of the coordination octahedron of the Ni atom is formed. Together with Cl1 -and Cl2 -anions, cations form supermolecules, which are packed into planar layers with a square cellular structure. The layers are linked by hydrogen bonds formed by crystalliza tion water molecules that are located between the layers.