Abstract. We study ultrathin quasicrystalline (QC) films as catalysts for the synthesis of carbon nanotubes (CNTs). To optimize the conditions for the synthesis of CNTs with single chirality, it is important to understand the effects of the catalyst on the chirality-selectivity. Among QC alloys found so far, an icosahedral Al--Cu--Fe alloy system with fivefold symmetry was tested for a catalyst in the synthesis of CNTs by alcohol catalytic-chemical vapor deposition (CCVD). Cross-sectional scanning electron microscopic images of the samples revealed that verticallyaligned CNTs were synthesized reproducibly. It implies that QC films have a significant catalytic activity for the synthesis of CNTs. Moreover, preliminary results of chirality-selectivity are obtained by means of resonance Raman scattering. It is suggested that Al--Cu--Fe ultrathin films are useful for the preferential synthesis of armchairtype CNTs, that is, QC nanoclusters play an important role as catalyst in alcohol CCVD.