Iron aluminides exhibit good resistance to high-temperature oxidizing and sulphidizing environments and have potential for structural applications at high temperatures under corrosive environments. In this study, an Fe-Al intermetallic compound was prepared by multi-layered roll-bonding of elemental Fe and Al foils. The process consisted of the accumulative roll-bonding (ARB) for making a laminated Fe/Al sheet and the subsequent heat treatment promoting a solid-phase reaction in the laminated Fe/Al sheet. Accumulated foils were rolled and bonded at room temperature or 573 K. A pulsed electric current sintering (PECS) process was used for the subsequent heat treatment. The microstructures produced at each processing stage were characterized by optical microscopy and scanning electron microscopy (SEM) equipped with energy-dispersive X-ray spectroscopy (EDS). Vickers microhardness testing was used for hardness determination. A homogeneous intermetallic compound of Fe3Al or FeAl could be obtained after the subsequent heat treatment for 1.8 ks at 873 K and for 3.6 ks at 1173 K.