The intermetallic compound Nb3Al is widely investigated because of its high temperature strength, superior superconductivity and relatively small density. As Nb3Al has an extremely high melting point and lack of deformability, it is impossible to prepare it by using the conventional metallurgy. In this study, a Nb-Al intermetallic compound was prepared by multi-layered roll-bonding of elemental Nb and Al foils. The process consisted of the accumulative roll-bonding (ARB) for making a laminated Nb/Al sheet and the subsequent heat treatment promoting a solid-phase reaction in the laminated Nb/Al sheet. Accumulated foils were roll-bonded at 573 K. The rolling reduction at 1 pass was ~50%, and the final rolling reduction at 4 passes was ~94%. A pulsed electric current sintering (PECS) process was used for the subsequent heat treatment. The microstructures produced at each processing stage were characterized by X-ray diffraction (XRD), optical microscopy and scanning electron microscopy (SEM) equipped with energy-dispersive X-ray spectroscopy (EDS). A homogeneous intermetallic compound of Nb3Al could be obtained after the subsequent heat treatment for 1.8 ks at 873 K and for 0.9 ks at 1673 K.