Aluminum-supported iron and cobalt (Fe-Co/Al2O3) bimetallic nano-sized catalyst has been synthesized by the sol-gel method. The average diameter of the Fe-Co/Al2O­3 catalyst was measured to be around 7 nm from SEM images. EDX measurements revealed that Fe-Co/Al2O­3 consists of 59.98% of Al, 20.00% of Fe, and 20.02% of Co by atomic weight. Multi-walled carbon nanotubes (MWCNT) were prepared with as-synthesized nanocatalyst from a commercial butane gas by the CCVD method at different reaction temperatures. TEM and XRD measurements revealed that Fe-Co/Al2O3 bimetallic nano-sized catalyst is beneficial to fabricating MWCNTs by the CCVD method. The highest yield of MWCNTs was obtained at 690°C.