The development of novel thermal barrier coatings (TBCs) by a 300 kW twin hybrid plasma spraying system was conducted as a case study of the integrated and comprehensive thermal plasma deposition technique, namely, the combination of thermal plasma powder spray (TP-PS) and the thermal plasma physical vapor deposition (TP-PVD). Microstructures of the coatings deposited from either vapor or melted droplets were tailored to compose peculiar functional layered Al 2 O 3 /YSZ and YSZ/YSZ coatings in the comprehensive deposition processes, aiming to meet the severe requirements of the next-generation TBCs. Even for the vapor deposition, ultrafast deposition rate over 150 µm/min was achieved. These results showed that the comprehensive spraying process has successfully integrated the potentials of different thermal plasma deposition techniques, and the effectiveness and flexibility of this process made it very promising to be applied in future coating industry.