Metal-semi organic NLO single crystal of Cadmium (II) dibromide L - Proline monohydrate (CBLPM) has been synthesized and the crystal was grown from solution by room temperature slow evaporation method. The crystal structure and cell parameters were refined by Rietveld refinement technique and confirmed that the metal-semi organic samples are in the orthorhombic system with space group P212121. The crystal structure of CBLPM is stabilized by intermolecular N–H…O, N–H….Br, O–H….O and O–H….Br hydrogen bonds. The water molecules serve as donors for the weak O–H⋯O and O–H⋯Br hydrogen bonds which link adjacent chains forming a three-dimensional structure. A Hirshfeld surface analysis suggests that the most significant contribution to the crystal packing is by H⋯Br contacts (26.2%). The complete vibrational features and electronic absorption spectra of the title compound were analyzed by FT-IR, FT-Raman and UV–visible spectra combined with density functional theory and time-dependent density functional computations. The second-order hyperpolarizability value of the molecule was also calculated at density functional theory method. The third-order nonlinear optical properties of the crystal were studied by Z-scan techniques using CW laser with wavelength 532 nm. The open aperture result exhibits the saturation absorption, which indicates that this material has potential candidate for optical limiting applications. © 2019 Elsevier B.V.