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Y2O3-doped BaZrO3 (BYZ) thin films were deposited by electrostatic spray deposition (ESD) technique. The effects of substrate temperature, precursor solution, flow rate, nozzle to substrate distance, voltage, and deposition time on the quality of the films have been studied. The microstructure, phase, and proton conductivities of the deposited BYZ thin films has been characterized by scanning electron microscopy (SEM), X-ray diffraction (XRD), and electrochemical impedance spectroscopy technique, respectively. The result has showed that ESD is an effective technique for thin film fabrications in both nano- and micro-scale electrochemical device.