Abstract: Catalyst particles with narrow size distribution were prepared on glass substrate by spin coating method. The surface morphologies of the films were controlled by varying the angular velocity, circumrotate time, and deoxidized temperature. By optimizing synthesis conditions, well-distributed catalyst particles could be obtained, most of which concentrate around 47~62 nm on the catalyst film. Vertically aligned carbon nanotubes were prepared on the above catalyst film by chemical vapor deposition(CVD). The samples were characterized by scanning electron microscope, transmission electron microscope and Raman spectroscope. The results indicate that spin coating is preferable to generally used dripping method in such aspects as producing substrates with low surface roughness, restricting the c