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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.

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In the asymmetric unit of the title salt, C6H9N2 +·C7H7O3S−, there are two independent 2-amino-6-methyl­pyridinium cations and two independent 4-methyl­benzene­sulfonate anions. Both cations are protonated at their pyridine N atoms and their geometries reveal amine–imine tautomerism. In the 4-methyl­benzene­sulfonate anions, the carboxyl­ate groups are twisted out of the benzene ring planes by 88.4 (1) and 86.2 (2)°. In the crystal, the sulfonate O atoms of an anion inter­act with the protonated N atoms and the 2-amino groups of a cation via a pair of N—H⋯O hydrogen bonds, forming an R 2 2(8) ring motif. These motifs are connected via N—H⋯O hydrogen bonds, forming chains running along the a-axis direction. Within the chains there are weak C—H⋯O hydrogen bonds present. In addition, aromatic π–π stacking inter­actions [centroid–centroid distances = 3.771 (2), 3.599 (2), 3.599 (2) and 3.497 (2) Å] involving neighbouring chains are also observed.

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