Single crystals of the organometallic material tetra(thiourea)copper(I) chloride (TTCC) were grown from aqueous solution. It is interesting to observe that Co2+-doping influences the efficiency of some of the physical properties of TTCC. Presence of Co2+ ions in the doped specimen is confirmed by energy dispersive X-ray spectroscopy (EDS) and chemical tests. FTIR studies reveal that the binding of thiourea with copper chloride occurs through sulphur. Doping results in reduction in the intensity of XRD peaks. SEMreveals that doping results in layered growth of the crystal. DSC confirms slight variations in the decomposition pattern. Mechanical stability of the doped specimen is much better than TTCC. Optical transparency is slightly enhanced by doping and a wide transmission in the visible region is observed. TTCC is non-linear optics (NLO) inactive and the second harmonic generation (SHG) efficiency is not influenced much by the added dopant.