It is essential to characterize the high-field properties of piezoelectric composites for their applications in ultrasonic transducers. This study involved the development of an experimental characterization system of piezoelectric impedance spectra and mechanical quality factors under high-field conditions to analyze the properties of PMN-PT piezoelectric single-crystal composites. The impedance spectra and mechanical quality factors of a [001]c-poled 0.69PMN-0.31PT single crystal/epoxy 1–3 composite disk with filling ratio φ = 0.4 under thickness resonance mode were tested at different driving voltages ranging from 1 to 120 Vpp to explore the influence of AC electric field on the material properties. By utilizing a theoretical approach, an evaluation was conducted on the variations in the material properties such as stiffness, permittivity, piezoelectric coefficient, and electromechanical coupling factor, along with respective loss factors. Our results suggest that as the AC electric field increases, the elastic modulus c33D and the mechanical quality factor Qm decrease, while the piezoelectric strain coefficient d33 and the electromechanical coupling factor kt increase. However, the dielectric coefficient ε33X does not show an obvious change in this field range. Furthermore, the elastic loss factor tanϕ, the dielectric loss factor tanδ33′, the piezoelectric loss factor tanθ33′, and the electromechanical coupling loss factor tanχt all increase, indicating that the loss of the piezoelectric composite becomes more evident as the AC electric field grows.