We present a simple technique for the calibration, prediction, and optimization of the optical modulation properties of a liquid-crystal display (LCD). The method is useful when there is no information about the internal fabrication parameters of the device (the orientation of liquid-crystal molecules, the twist angle, or the birefringence of the material). A complete determination of the LCD Jones matrix is accomplished by means of seven irradiance measurements for a single wavelength. This technique only requires two linear polarizers and one quarter-wave plate. Once the Jones matrix has been calibrated, the amplitude, phase, and polarization modulation response can be predicted. Therefore, it can be optimized through the control of the polarization configuration. The validity of the proposed method is experimentally probed. Finally, we present a particular application to produce phase-only modulation.