In the present work, successful growth of alpha- and gamma-glycine single crystals using cesium carbonate (Cs2CO3) as an additive has been reported. The powder XRD study confirms that the grown 0.2 M cesium carbonate added glycine crystal has alpha-glycine crystal morphology and it crystallized in a monoclinic crystal structure with a space group of P21/n. In a similar manner, the PXRD patterns recorded for 0.4, 0.6, 0.8 and 1 M concentrations of cesium carbonate added glycine crystals and the obtained PXRD patterns authenticated that the harvested grown crystals belong to hexagonal crystal system with space group P31. The variation of dielectric constant and dielectric loss for the gamma-glycine single crystal was carried out as a function of frequency and the results were discussed in detail. The transmittance spectrum shows that the grown alpha- and gamma-glycine crystals had an extensive optical transparency window in the entire spectrum especially in visible region. The band gap varies from 4.59 to 6.01eV. The positive photoconducting nature of the grown gamma-glycine single crystal in the presence of cesium carbonate was studied by the photoconductivity study. The second harmonic generation (SHG) for the prepared gamma-glycine single crystals was studied by using Kurtz and Perry powder technique with Nd-YAG laser. The result shows that the prepared gamma-glycine single crystals exhibit enhanced second harmonic conversion efficiency and it proves that these crystals are an alternate to KDP crystal in optoelectronic devices and NLO applications.