Piezoelectric plates can provide low-frequency transverse vibrational displacements and high-frequency planar vibrational displacements, which are usually uncoupled. However, piezoelectric shells can induce three-dimensional coupled vibrational displacements over a large frequency range. In this study, three-dimensional coupled vibrational characteristics of piezoelectric shells with free boundary conditions are investigated using three different experimental methods and finite element numerical modeling. For the experimental measurements, amplitude-fluctuation electronic speckle pattern interferometry (AF-ESPI) is used to obtain resonant frequencies and radial, lateral, and angular mode shapes. This optical technique utilizes a real-time, full-field, non-contact optical system that measures both the natural frequency and corresponding vibration mode shape simultaneously. The second experimental technique used, laser Doppler vibrometry (LDV), is a pointwise displacement measurement method that determines the resonant frequencies of the piezoelectric shell. An impedance analyzer is also used to determine the resonant frequencies of the piezoelectric shell. The experimental results of the resonant frequencies and mode shapes for the piezoelectric shell are verified with a numerical finite element model. Excellent agreement between the experimental and numerical results is found for the three-dimensional coupled vibrational characteristics of the piezoelectric shell. It is noted in this study that there is no coupled phenomenon at low frequencies over which radial modes dominate. However, three-dimensional coupled vibrational modes do occur at high resonant frequencies over which lateral or angular modes dominate.