A new hydrogen bonded Cobalt(II) Schiff base complex, N'-(pyridine-4-carboxaldehyde) isonicotinoylhydrazone Cobalt(II), has been synthesized from isoniazid and pyridine-4-carboxaldehyde and characterized by IR spectroscopy, 1 H-NMR, elemental analysis, TGA and single crystal X-ray structure determination. X-ray crystal structure analysis shows an octahedral complex with a metal centre coordinated to two ligand molecules through the pyridine nitrogen atoms and four water molecules and containing two nitrate groups as counter ions. The complex crystallizes in the monoclinic crystal system and P2(1)/n space group. The unit cell dimensions are: a = 7.2108(4) Å, b = 16.6020(9) Å, c = 13.0389(6) Å, α = 90˚, β = 103.972(4)˚, γ = 90˚. The molecule is symmetrical about the cobalt centre as observed from the 1 H-NMR and 13 C-NMR and confirmed by the single crystal X-ray structure of the complex. Thermogravimetric analysis shows two steps decomposition of the complex to leave a metal oxide residue. The title compound is expected to be biologically active as one of the precursors (isoniazid) is a therapeutic agent with well-established clinical applications.