The effects of deposition parameters and NH3 pretreatment on the size and distribution of Pd catalytic particles and subsequently their effects on the characteristics of the synthesized carbon nanotubes (CNTs) were systematically investigated. It was found that the size of Pd particles decreases and the particle density (total number of Pd particles per unit area) increases as the Pd film thickness decreases. Moreover, pretreatment, of Pd film in NH3 gas promotes smaller Pd particles and higher particle density which is beneficial for CNT growth. The CNTs were synthesized by thermal chemical vapor deposition at 750 degrees C using methane (CH4) as the carbon source, and a mixture of Ar/H-2 (80 vol %: 20 vol %) as a carrier gas with NH3 serving as a processing reagent. The incorporation of NH3 in CNT synthesis, per the specific pretreatment of catalytic film, has a distinct effect on the size and morphology of CNTs produced: The interrelation between processing, structure and emission behavior of CNTs produced with different synthesis conditions was examined by scanning electron microscopy, transmission electron microscopy, Raman spectroscopy, and field emission measurements. (c) 2005 American Vacuum Society.