Materials with favorable nonlinear optical properties receive more attention in advanced optical technology. This study aims to design, synthesize, and characterize a novel single crystal with exceptional third-order nonlinear optical (NLO) properties. Utilizing the solvent evaporation method a single crystal of 1-methyl-2[2-(4-ethylphenyl)vinyl]pyridinium iodide (EMPI) was obtained with high crystallinity. The crystal structure of the EMPI was determined through Single Crystal X-ray diffraction (SCXRD), confirming its atomic arrangement and its purity was verified using the CHN elemental analysis. Nuclear Magnetic Resonance (NMR) and Fourier Transform Infrared (FT-IR) spectroscopy confirmed the molecular composition (C16H18) and functional groups of the EMPI. Hirshfeld surface analysis was employed to elucidate the intermolecular interactions in the EMPI crystal. The optical characteristics of the EMPI crystal were evaluated through the UV-Vis-NIR spectroscopy and Photoluminescence (PL) analysis, revealing its remarkable 80% transparency in the visible range and suitability for green light-emitting diodes. AFM and etching analysis affirmed that EMPI crystal has a smooth surface with fewer dislocations. The Z-Scan analysis demonstrates the third-order nonlinear optical performance and the optical limiting capabilities of the EMPI crystal, highlighting its potential as a key material for advancing optoelectronic devices and optical protection systems.