Dye can induce positive change in crystal. Pure and xylenol orange-dyed triglycine sulphate (TGS) large single crystals (> 14 cm2) were grown by solution technique in which dye inclusion pattern along preferred crystallographic planes were visible. Rietveld refinement was used to confirm monoclinic phase with space group P21 in XRD analyses. The crystallite size of both grown crystals were calculated by Scherrer method. In FTIR and Raman analyses, all the observed functional groups were explained. Thermal stability of dyed TGS crystal was increased. UV–Vis–NIR spectra showed that grown crystals were highly transparent with the lower cut off at 230 and 228 nm for pure and dyed crystals, respectively. The characteristics luminescence properties, including hyperluminescence and additional luminescence nature in dyed crystal, were explained. Pure TGS fell in violet region which shifted in blue region in CIE diagram after dyeing. Changes in PL, Raman, UV–Vis and thermal behavior due to dye doping established the TGS crystal as a better candidate for optical applications.