Ga-doped ZnO (GZO) transparent conductive oxide thin films were deposited on flexible polyethersulphone (PES) substrates by radiofrequency sputtering at room temperature. With the addition of an optimized 100-nm-thick ZnO buffer layer, the transmittance, carrier concentration, Hall mobility, and resistivity of GZO films improved from 88.3 to 94.45%, −2.89 × 10 21 to −3.39 × 10 21 cm −3 , 1.76 to 7.97 cm 2 /V-s, and 1.32 × 10 −3 to 2.201 × 10 −4 -cm, respectively. The higher surface energy (49.85 mJ/m 2 ) of the 100-nm-thick ZnO layer deposited on the PES substrate compared to those of a bare PES substrate and ZnO layers of other thicknesses deposited on PES substrates is likely responsible for the superior GZO quality obtained with the GZO/100-nm-thick ZnO buffer/PES structure. Moreover, the best adhesion at the GZO surface was observed for the GZO/100-nm-thick ZnO buffer/PES structure based on it having the highest surface energy (67.33 mJ/m 2 ). The GZO/100-nm-thick ZnO buffer/PES structure thus has potential to replace the GZO/PES structure for use in flexible transparent optoelectronic devices.Transparent conductive oxide (TCO) thin films have a high carrier concentration, high mobility, and low resistivity in the visible light region, and are thus widely used for organic light-emitting diodes (OLEDs), 1 solar cells, 2 oxide thin-film transistors, 3 memory devices, 4 and touch panels. 5 Among TCO films, indium tin oxide (ITO) is widely used for industry applications due to its excellent resistivity (ρ ∼ 1 × 10 −4 -cm) and high transparency (about 85% in the visible region). However, indium is expensive and toxic. IIIA-elementdoped ZnO, such as ZnO:Al 6 and ZnO:Ga, 7,8 has been found to be a promising material to replace ITO because of its lower cost, lower deposition temperature, and lower toxicity. Compared to the covalent bond length of Zn-O, the variations in the covalent bond length of Al-O and Ga-O are 0.13 and 0.05 Å, respectively, and thus GZO has a smaller lattice deformation than that of AZO. Additionally, Ga is less reactive to oxidation than Al during the deposition. 7 Therefore, GZO is more suitable than AZO to replace ITO.Compared with glass substrates, flexible substrates have a rougher surface, and thus higher resistivity. It is known that the resistivity of flexible-substrate-based devices can be lowered by utilizing a GZO/metal/GZO structure. However, this structure increases the cost of the deposition process. Several reports have suggested that a GZO/ZnO buffer structure could enhance TCO properties by reducing the film roughness and improving crystallization. 9 To our best knowledge, there has been only one study on GZO film deposited on flexible substrates with a buffer layer using the radio-frequency (RF) sputter deposition method. Gong et al. reported that the configuration of GZO/ZnO on polycarbonate (PC) substrates could be realized and that the optimal parameters of the ZnO buffer layer could be obtained according to the Taguchi experimental design. 10 The lowest electrical resistivi...