Metallic substances are favored for storing and transporting spent nuclear fuels (SNFs) due to their thermal stability, mechanical strength, and corrosion resistance. Adding gadolinium (Gd) significantly enhances neutron shielding, improving efficiency with reduced thickness and dimensions. In this study, Al–Gd2O3 metal nanocomposites were synthesized using powder-processed mechanical milling. The crystal structure features of (100-x)Al-x%Gd2O3 samples with varying percentages of Gd2O3 (5 %, 10 %, and 15 % by weight) were analyzed by X-ray diffraction. Microstructural properties were studied using scanning and transmission electron microscopy (SEM and TEM). The synthesized composites' neutron and γ-radiation shielding characteristics were investigated theoretically using the MCNP6.2 transport code. Analysis of the XRD data revealed prominent peak shifts with increased milling time, indicating reduced particle sizes. Differential scanning calorimetry (DSC) indicated Gd2O3-induced changes in temperature behavior, and the Vickers microhardness tests demonstrated enhanced mechanical strength with increasing gadolinium concentration. Improved neutron radiation shielding was observed with higher Gd2O3 content. Our study highlights the potential of Gd2O3-enriched metal matrix composites for advanced industrial applications.