Thermal barrier coatings (TBCs) have been widely used in gas turbine engines to protect the underlying metal from high operating temperature so as to improve the durability of the components and enhance the engine efficiency. However, since the TBCs always operate in a demanding high-temperature environment of aircraft and industrial gas-turbine engines, a better understanding of this complex system is required to improve the durability and reliability. The objective of this study is to investigate the effects of surface modification for the NiCoCrAlY bond coats on the thermal cycling lifetime and failure characteristics of TBCs. Parameters of modification for the bond coats included as-sprayed, barrel-finished, hand-polished and pre-oxidation heat treatment at 1100[degrees]C in P=10O2-8 atm up to 4 hours, carried out prior to the electron beam physical vapor deposition (EB-PVD) of ZrO2-7wt% Y2O3 (7YSZ) ceramic topcoat. The resulting characteristics of the bond coat and the thermally grown oxide (TGO) scale were initially documented by surface roughness, phase constituents of the TGO scale, and residual stress of the TGO scale. The thermal cycling test consisted of 10-minute heat-up to 1121°C, 40-minute hold at 1121°C, and 10-minute forced air-quench. As-coated and thermally-cycled TBCs were characterized by optical profilometry (OPM), photo-stimulated luminescence spectroscopy (PSLS), optical microscopy, scanning electron microscopy (SEM) equipped with energy dispersive spectroscopy (EDS), and scanning/transmission electron microscopy (TEM/STEM) equipped with high angle annular dark field (HAADF) and X-ray energy dispersive spectroscopy (XEDS). TBC specimens for TEM/STEM analysis were prepared by focused ion beam (FIB) in-situ lift-out (INLO) technique. Superior thermal cycling lifetime was observed for TBCs with as-sprayed bond coats regardless of pre-oxidation heat treatment, and TBCs with hand-polished bond coats only after pre-oxidation heat treatment. With pre-oxidation heat treatment, relative photostimulated luminescence intensity of the equilibrium α-Al2O3 increased. Thus, the improvement in TBC lifetime can be correlated with an increase in the amount of α-Al2O3 in the TGO scale, given a specific surface modification/roughness. The lifetime improvement due to pre-oxidation was particularly significant to TBCs with smooth hand-polished bond coats and negligible for TBCs with rough as-sprayed bond coats. Spallation-fracture paths depended on the lifetime of TBCs. Premature spallation of TBCs occurred at the interface between the YSZ and TGO. Longer durability can be achieved by restricting the fracture paths to the TGO/bond coat interface. Small particulate phase observed through the TGO scale was identified as Y2O3 (cubic) by diffraction analysis on TEM. While small addition of Y in the NiCoCrAlY bond coat helps the adhesion of the TGO scale, excessive alloying can lead to deleterious effects.