Electrophoretic displays (EPDs) based on photonic crystals show great potential due to their reduced eye fatigue and low power consumption. However, the current image quality and service life of this system still face great challenges. In this work, we fabricated a new kind of electrically responsive photonic crystal (ERPC) device based on PSMA@SiO2 liquid colloidal crystals (LCCs) for EPDs. By introduction of the PSMA core with lower density and higher refractive index, the suspension stability and color saturation of PSMA@SiO2 LCCs were greatly enhanced compared with those of bare SiO2 LCCs. The PSMA@SiO2 LCCs showed brilliant colors, wide color tuning range (∼200 nm), and good reversibility under low voltages (<4 V). Interestingly, the transparency of PSMA@SiO2 LCCs could also be obviously regulated by an electric field, which was different from the traditional ways that change the thickness of PCs or contrast of refractive index (Δn) between the nanospheres and matrix. This transparency modulation offered a novel idea for the transmittance control of smart windows. As a proof of concept, we fabricated a new type of patterned ERPC device to demonstrate their potential in electrophoretic displays and smart windows with controllable transmittance under an electric field.