A novel method of forming catalyst particles, on which carbon nanotubes grow based, on a substrate with increased uniformity, and a method of synthesizing carbon nanotubes having improved uniformity are provided. A catalytic metal precursor solution is applied to a substrate. The applied catalytic metal precursor solution is freeze-dried, and then reduced to catalytic metal. The method of forming catalyst particles can minimize agglomeration and/or recrystallization of catalyst particles when forming the catalyst particles by freeze-drying the catalyst metal precursor solution. The catalyst particles formed by the method has a very uniform particle size and are very uniformly distributed on the substrate.