The ∼45mm long and 20mm diameter large single crystals of the l-proline cadmium chloride monohydrate (LPCCM) has been first time grown by the unidirectional Sankaranarayanan–Ramasamy (SR) method in aqueous medium. The crystal structure has been confirmed by powder X-ray diffraction. Vibrational frequencies of the grown single crystals have been identified by using FT-Raman spectroscopy. The crystalline perfection was assessed by high-resolution X-ray diffractometry (HRXRD) and found that the quality of the grown single crystal is quite good. The laser damage threshold (LDT) was measured using single shot method and found to be 4.747GWcm−2 and the measured second harmonic generation (SHG) efficiency was found to be 2 times than that of KDP. The UV–Vis-NIR spectroscopic study revealed that the grown single crystal has good optical transparency. The crystal has shown yellow fluorescence. The dielectric studies have been carried out over the frequency range of 10mHz to 10MHz.