Optically good-quality, organometallic bulk single crystal of guanidinium chlorochromate (GCC) was fruitfully grown by Sankaranarayanan–Ramasamy (SR) method. Translucent (− 1 − 1 2) aligned unidirectional bulk single crystals of diameter 20 mm and length maximum up to 48 mm were grown over the growth period of 23 days with growth rate of 1 mm/day by the SR method. Optical studies reveal very high transmission of the crystal along the growth axis. Microhardness measurement along the growth axis enounces high mechanical stability of the crystal. Laser damage threshold value of 1.11 GW/cm2 has been determined using Q-switched Nd:YAG laser radiation for GCC single crystal and reported for the first time. The second harmonic generation (SHG) of GCC crystal was investigated by the SHG Maker fringes technique. The refractive index and birefringence value of GCC crystal were found. © 2020, The Optical Society of India.