Polyamide 66 (PA66) is a material with high wear resistance, toughness, and heat resistance. However, low stiffness and thermal deformation during thermal processes define applications in many conditions. Carbon powder efficiently enhances stiffness and reduces thermal deformation, which makes up defects of plastic materials. However, forming a composite with fused deposition modeling (FDM) that accumulates material to a specified location by melting plastic filaments is limited, including fluidity and viscosity to form normally. In this paper, filaments of polyamide 66 (PA66) reinforced with carbon powder were produced. Digimat was used to analyze the composite material properties of different carbon contents and predict the proper carbon content. Then, the material properties were imported to ANSYS software to simulate the thermal deformation of the workpieces during processing. It was verified that adding carbon powder is helpful in decreasing thermal deformation. Comparing experiments and simulations, we found that 20% carbon mass fraction was best, and that thermal deformation was minimal at 240 °C nozzle temperature while hot bed temperature was 90 °C. The optimal ratio of extrusion speed to filling speed was 0.87, and the best aspect ratio was 0.25.