In present work, the pure and brilliant green dye doped single crystals of nonlinear optical zinc tris(thiourea) sulfate have been grown for the first time using slow evaporation solution technique from their aqueous solutions. The powder X-ray diffraction and FT-Raman spectroscopic investigations were carried out to confirm and identify the crystal structure and vibrational modes, respectively. The strong effect of dye on crystals morphology is observed. For optical band gap analysis the diffused reflectance was measured. Two absorption bands were observed in the diffused reflectance spectrum centered at *425 and 627 nm due to brilliant green dye. Room temperature PL study with 310 nm excitation show noticeable enhancement in UV-blue emission band centered at 348 nm due to dye doping and also the enhancement in violet-blue emission centered at 420 nm was observed. Mechanical strength was also found to be enhanced with doping. All the results show that the properties of ZTS crystals are enriched due to dye doping and can be applied in optoelectronic devices.