Single-walled carbon nanotubes (SWNTs) were synthesized using size-controlled catalyst nanoparticles created by the pulsed laser ablation method. Specifically, the alloy particles (Co/Mo or Co/Pt) were prepared by ablation of the target alloy materials in an inert gas atmosphere. Size selection was performed using a differential mobility analyzer (DMA). The obtained nanoparticles were deposited on a quartz substrate from which SWNTs were grown by the alcohol catalytic CVD (ACCVD) technique that was developed by the authors’ group. AFM and Raman scattering analysis revealed that SWNTs were successfully synthesized. It seems the Co/Mo alloy catalyst was more effective for the synthesis of SWNTs than the Co/Pt catalyst, though this is a preliminary result to be further investigated.