Cyclohexylammonium 4-nitrobenzoate (CYH4NBA) organic nonlinear optical material was crystallized using slow evaporation solution growth method and characterized by elemental analysis, single crystal X-ray diffraction, thermal analysis and dielectric studies. The functional group and molecular structure are identified by FT-IR and FT-NMR analyses. UV-Vis-NIR spectrum shows the cutoff wavelength is at 263.24 nm. It is compared with the value (259.83) calculated by time-dependent density-functional theory calculation. HOMO-LUMO energy difference and molecular electrostatic potential surface were investigated using density-functional theory calculations. The optical limiting phenomena, moderate melting point (160 degrees C) and large third-order nonlinear optical susceptibility (2.58 x 10(-6) esu) suggest that CYH4NBA is favorable for optical limiting applications.