The development of novel thermal barrier coatings (TBCs) by a high-power twin hybrid plasma spraying system was conducted as a case study of the integrated and comprehensive thermal plasma deposition technique. Characteristic microstructures deposited from either vapor or melted droplets were tailored to compose peculiar functional layered Al2O3/YSZ and YSZ/YSZ coatings in the comprehensive deposition processes, aiming to meet the severe requirements of the next-generation TBCs. The effectiveness and flexibility of this process made it very suitable to integrate the potentials of different thermal plasma deposition techniques, namely, the thermal plasma powder spray (TP-PS) and the thermal plasma physical vapor deposition (TP-PVD).