Two supramolecular Co(II)-based coordination compounds have been harvested from dithiolate and di-carboxylate ligands. They have been structurally characterized by FT-IR, elemental analysis, and sin-gle crystal X-ray diffraction. Salt 1 consists of two ([tris (2-aminoethyl) amine Co] 1,1-dicyano-2,2-ethylenedithiolate)+ per thiosulphate ion linked through intermolecular hydrogen bonds. Compound 2 , (pyridine-2,6-dicarboxylate)2Co-5H2O -Co).2H2O, is stabilized by intramolecular O -H center dot center dot center dot O hydrogen bonds, building ribbons that propagate along the  direction in the crystals. From HS analysis, it is observed that the major non-covalent interactions present in 1 are C -H center dot center dot center dot O, N -H center dot center dot center dot N, N -H center dot center dot center dot S, and N -H center dot center dot center dot O hy-drogen bonds, which play an important role in stabilizing the crystal structure. In 2 , out of all the non -covalent interactions, O center dot center dot center dot H/H center dot center dot center dot O interactions have major contributions to stabilize the crystal structure. Theoretical investigation on the molecular structures of the crystals also revealed that the major stabi-lizing factor for 1 is H-bonding along with pi-pi stacking while that for 2 is co-ordinate bond between water and cobalt(II) ion. Direct current variable-temperature magnetic susceptibility measurements car-ried out on polycrystalline samples of 1 and 2 in the temperature range of 1.8-300 K shows the presence of magnetic anisotropy of the cobalt(II) ion in 1 and weak intermolecular exchange in 2 . Further, both the compounds 1 and 2 are found to be highly efficient water reduction catalysts in terms of per Co turn-over-numbers at lower concentrations.(c) 2023 Elsevier B.V. All rights reserved.