Guanidinium trichloroacetate (GTCA), a novel organic single crystal was grown by a slow evaporation technique. The single crystal X-ray diffraction study revealed that the GTCA crystal belongs to tetragonal crystal system with the space group P41. From the linear optical studies, the lower cut-off wavelength of grown crystal was found at 257[Formula: see text]nm. The luminescent study showed that the GTCA crystal has high degree of luminescence. The single shot laser damage threshold of grown crystal is found to be 2.6[Formula: see text]GW/cm2. The nonlinear refractive index, absorption coefficient and third-order susceptibility were estimated by Z-scan technique. The two independent tensor coefficients [Formula: see text] of the dielectric permittivity were calculated.