In the present study, pure and LL-cystine (LC) doped zinc thiourea sulphate (ZTS) crystals have been grown by slow evaporation solution technique at ambient temperature. The powder X-ray diffraction (XRD) analysis has been carried out to identify the shifts in peak positions and structural parameters of grown crystals. The incorporation of LC in ZTS crystal has been qualitatively analyzed by means of Fourier transform infrared (FTIR) spectroscopic study. In UV-visible studies, the influence of LC on optical transparency, bandgap and various optical constants of ZTS crystal have been investigated to explore various optical applications. The thermal stability of LC doped ZTS crystal has been determined by means of differential scanning calorimetry (DSC) analysis. The hardness behavior and hardness number of grown crystals have been comparatively evaluated by employing the Vicker’s microhardness test. The dielectric study of pure and LC doped ZTS crystal has been carried out at different temperature. In Kurtz–Perry powder technique, the second harmonic generation (SHG) efficiency of LC doped ZTS crystal is found to be 1.16 times that of ZTS crystal.