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Al-doped ZnO (AZO) is a promising candidate as a transparent conducting electrode. However, the electrical properties of AZO deteriorate greatly after exposing it to excessive heat. This limits the applications of AZO in devices that experience a demanding operation environment. It has been shown that a ZnO cap layer with proper morphology is capable to dramatically improve the thermal stability of AZO. However, the detailed mechanism is not yet clear. A comparison study of the electrical properties of AZO with a ZnO cap layer prepared by magnetron sputtering (MS) at low substrate temperature (70 °C) and chemical vapor deposition (CVD) at high substrate temperature (600 °C) indicates that MS-prepared ZnO is much less effective in protecting AZO from an oxidizing environment under elevated temperature than the CVD-prepared ZnO. The morphology and crystal structures of two types of ZnO/AZO, investigated by a scanning electron microscope and x-ray diffraction, are relatively similar, whereas the atomic structures (e.g., defects) revealed by Raman spectroscopy are rather different. The results suggest that it is difficult to improve the thermal stability of electrical properties of AZO without a proper restructuring process and a ZnO cap layer that could sacrifice its own structural order. The discoveries offer a novel approach to improve the performance of other transparent conducting oxides. [ABSTRACT FROM AUTHOR]