In this paper, indium (In) films were deposited on glass substrates using DC sputtering method. Multiwalled carbon nanotubes (MWCNTs) and dispersant were dissolved in alcohol, and the mixed solution was deposited on the In films using the spray method. The bi-layer MWCNTs-In2O3 films were annealed at different temperatures (from room temperature to 500°C) in O2 atmosphere. The influences of annealing temperature on the characteristics of the bi-layer MWCNTs-In2O3 films were investigated by scanning electron microscopy, X-ray diffraction pattern, Fourier transform infrared (FT-IR) spectroscopy, and Raman spectroscopy. A separative extended-gate field-effect transistor (EGFET) device combined with a bi-layer MWCNTs-In2O3 film was constructed as a pH sensor. The influences of different annealing temperatures on the performances of the EGFET-based pH sensors were investigated. We would show that the pH sensitivity was dependent on the thermal oxygenation temperature of the bi-layer MWCNTs-In2O3 films.