Radiation safety and protection is a subject of major concern for all communities because of the biological damage caused by different radiation sources. Therefore, the purpose of this study is aimed to synthesize two different thin films from a newly synthesized N-Al2O3@Pb(II)-2,4-DiNA nanocomposite which was prepared by the direct chemical coupling of nano-aluminum oxide (N-Al2O3) with Pb(II)-2,4-dinitroaniline complex. The synthesized materials were characterized by FT-IR, thermogravimetric analysis (TGA), scanning electron microscope SEM, and elemental composition by energy-dispersive X-ray (EDX). The two thin films were assembled by the encapsulation of N-Al2O3@Pb(II)-2,4-DiNAnanocompositeinto hydrolyzed polyurethane and hydrolyzed polyvinyl chloride. Electron spin resonance (ESR) measurements have been used to investigate the newly prepared nanocomposite and thin films before and after gamma irradiation. Gamma spectroscopy, Phy-X software, and SRIM (stopping and range of ions in matter) Monte Carlo simulation code are aimed to apply and investigate radiation shielding efficiency of films for gamma/x-ray, protons, alpha, and thermal neutrons. The gamma shielding characteristics, mass stopping power (MSP), and range for both proton (H-ions) and alpha (He-ions) were also calculated. In addition, the SRIM code’s subroutine TRIM was used to predict the damage production and atomic displacements per atom (dpa) caused by the interaction of high-energy H-ions (proton) and He-ions (alpha) with the studied samples. The data obtained the good radiation shielding effect of the prepared thin films and their possible use as radiation shielding materials for X-rays and low gamma energy.