Optical materials and organic and nonlinear molecules are the leading materials that exhibit semiconducting properties that are useful for industrial purposes in terms of their optical and electronic properties. These active organic materials developed into films are of vital importance in terms of their molecular structure, molecular properties, and electronic and optical properties compared to inorganic materials. The present article focuses on the development of thin films with the synthesis of Schiff base of 4-hydroxy benzaldehydes and substituted anilines to obtain target compounds using the green synthesis method. The formation of the Schiff base compounds was confirmed by spectral methods, infrared spectroscopy, ultraviolet spectroscopy, and proton NMR. Powdered XRD provide useful information of structure, composition and crystalline proximity of the synthesized Schiff base compounds. The optical properties of the refractive index and dielectric constant were confirmed by spectroscopic ellipsometry studies. Computational studies were performed using the Gaussian 16 package with the B3LYP method basis set 6-311++** for all molecular compounds to confirm the molecular structures, optimized geometry, and electronic and optical properties.The insights of these properties are best visualized in terms of quantum mechanical descriptors that occur due to changes in electron density. Studies of these Schiff base compounds with nitro groups proved to exhibit optical properties and behave as excellent organic semiconducting materials with an energy gap of 3.08 eV ; refractive index of 2.074, and dielectric constant of 4.303.