The thermal insulation properties of thermal barrier coatings (TBCs) can be significantly improved with increasing the coating thickness. However, due to the weak bonding of high-thickness TBCs, the resulting low reliability and short lifetime greatly limits their application under some severe operating conditions. In this study, a novel and high-efficiency synchronous dual powder feeding method is used to deposit a series of gradient NiCoCrAlY/YSZ coatings with millimeter level thickness. The tensile bonding strengths and residual stress state of coatings are evaluated in order to explore the effect of thickness on the bonding strength of coating. The results suggested that, due to some micro-convex structure at the “GC/TC” interface and inside “GC” layer, the bonding strength of 1000-μm-thickness gradient NiCoCrAlY/YSZ TBCs with the 4:6 and 2:8 hybrid ratios is over 44 MPa compared to the common TBCs. The fracture position gradually shifts from NiCoCrAlY bond coat to NiCoCrAlY/YSZ transition zone and finally to the YSZ top coat owing to the different position of residual stress concentrations. After thermal cycling tests, the 1000-μm-thickness gradient coating exhibits a higher thermal cycling life. Some coarse cracks initiate and propagate at the bottom region of TBCs, which is mainly due to thermal expansion mismatch stress that finally results in the failure of the gradient coating between the “BC” layer and the substrate.