We developed and adequately characterized the triglycine sulfate family crystals doped with specific molar percent of cobalt phosphate, TGS:PCo (9%). The crystals were grown by slow evaporation technique and the growth rates of different crystallographic planes are rather faster in comparison with the plane growth rates of pure TGS crystals. The introduction of Co 2+ ion as an active optical element to the structure of TGS crystal leads to optimization of some parameters such as optical quality, stability at ambient condition, Curie temperature, stronger Raman peaks, etc. Three new peaks at 460, 620 and 1368 cm −1 were observed in the dispersive back scattering Raman spectra of the grown TGS:PCo (9%) crystal in comparison with the pure triglycine sulfate crystal.