The present report describes the catalytic activity of mechanically activated nano quasicrystalline Al65Cu20Fe15 and related nano crystalline Al50Cu28Fe22 for the synthesis of carbon nanotubes (CNTs). CNTs are synthesized by catalytic decomposition of ethanol through nano quasicrystalline Al65Cu20Fe15 and related crystalline Al50Cu28Fe22 alloys as a catalyst. The synthesized multi-walled CNTs exhibits tube diameter ranging from 5 to 25 nm. The synthesized CNTs are characterized by scanning and transmission electron microscopy. It is found that Al65Cu20Fe15 nanoquasicystal shows better catalytic behaviour as compared to nano-crystalline Al50Cu28Fe22 alloys for decomposition of ethanol during the synthesis of multi-walled CNTs.