This paper presents an investigation into the plume characteristics of composite propellants fabricated by polytetrafluoroethylene (PTFE) filled with different carbon additives (nano-carbon powder, graphite, and graphene) under laser irradiation in a vacuum environment. The dynamic plumes generated by the laser ablation of different modified propellant samples were captured using a high-speed camera, and the feature parameters of the plumes were extracted by image processing. The results indicated that doping carbon particles in PTFE enhanced the quality of the plasma plumes. The plume area increased up to a certain value and then stabilized, while end of plume clusters remained for a short time. Further analysis revealed that the propellant sample doped with graphene exhibited the maximum plume length and expansion rate, whereas the propellant sample doped with nano-carbon demonstrated the largest plume area. Moreover, a higher graphene doping ratio promoted greater plume length, expansion speed, and plume area. However, when the doping ratio exceeded 3%, the gain of the plume parameters gradually became saturated, and the optimal doping ratio appeared to be 5%.