Aluminum and its alloys, such as Al–15Fe, Al–10Fe, and Al–5Fe, possess a unique blend of mechanical properties attributed to the development of intermetallic phases. These alloys are formed through the metallurgical casting process, where aluminum reacts chemically with iron. Renowned for their outstanding mechanical and physical characteristics, including corrosion resistance, high strength, thermal stability, and low density, Al–Fe intermetallic alloys find extensive applications across industries such as automotive, aerospace, chemical, medical, and electronics. This study involves the synthesis of Al–Fe intermetallic alloys through metallurgical casting using an induction furnace, supported by molecular dynamics simulations. The mechanical properties, including yield strength and hardness, were systematically assessed with varying iron content in the alloys. Results indicate a significant enhancement in these properties with increasing Fe content. Furthermore, structural phase analysis and the formation of intermetallic compounds were examined using optical microscopy and atomic-level investigations, offering a detailed understanding of the microstructural and intermetallic phase distribution within the materials.