The Fe₂VAl alloy was produced through the mechanical alloying and the pulsed current sintering process to clarify the optimum milling condition for obtaining homogeneous Fe-Al based intermetallic compounds. The homogeneity of the milled powder was evaluated from the absolute value of Seebeck coefficient, |S|, of the thermoelectric Fe₂VAl alloy. It used to be that the synthesis of the homogeneous Fe₂VAl powder yields after the milling for 720 ks in the case of using conventional planetary ball milling process. On the contrary, under the modified milling conditions optimized in this study, which were the orbital speed of 900 rpm and the inversed rotating speed of 300 rpm, enabled to cut down the milling time can be shortened to 10.8 ks to provide the satisfactory Fe₂VAl powder. The |S| values of Fe₂VAl alloy sintered from the powder produced through the optimum milling were comparable to those of alloys fabricated by a conventional melting technique.