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To widen the measuring range of liquid film thickness, a new approach combining resistance-based method and ultrasound-based method is proposed. A new type of electrical-acoustic composite sensor was designed, and a numerical model was established to optimize the electrode structure parameters. The optimal electrode parameters were determined with the sensitivity and linearity as optimization specifications. The validity of the joint measurement approach was verified by the liquid film thickness measurement experiment. It has been demonstrated that: the coaxial metal electrode is suitable for measuring a thinner liquid film, and the relative error ranges from -4.93% to 5.35% in the thickness range of 2.4 mm to 4.4 mm; the ultrasonic probe is more suitable for measuring a thicker liquid film, and the relative error ranges from -3.68% to 2.20% in the thickness range of 3.4 mm to 10.0 mm. The measurement range of the two methods can be expanded and the reliability of the measurement results can be improved through the combination of the resistance-/ultrasound-based methods. The proposed method has the advantages of wide measurement range, non-intrusive, fast response, high accuracy and sensitivity, and good safety, which can be widely used in industrial production and laboratory research applications.