The structure of amorphous CNₓ thin films has a variety of chemical bond, and studies on these bonds ratios are very important because these ratios determine the appropriate technical use of these films. Therefore, this paper aim to investigate the relation between the conditions of preparation (deposition pressure) of a-CNₓ thin films prepared using PLD (Pulsed Laser Deposition) method and the film's structure. Results shown that the deposition pressure variation does not affect the concentration in the same manner for all bonds in the film. Moreover, the sp² cluster size and the order degree are related to the numerical value of the deposition pressure.