This paper reports the synthesis of yellow-charged particles with a core–shell structure by modifying yellow pigment 181 particles using an ionic liquid under the sol–gel and grafting methods. The core–shell particles were characterized using various methods, including energy-dispersive X-ray spectroscopy, Fourier-transform infrared spectroscopy, colorimetry, thermogravimetric analysis, and others. The changes in zeta potential and particle size before and after modification were also measured. The results demonstrate that the surface of the PY181 particles was successfully coated with SiO2microspheres, resulting in weak color change but increased brightness. The shell layer also caused an increase in the particle size. Moreover, the modified yellow particles exhibited apparent electrophoretic response, indicating improved electrophoretic properties. The core–shell structure significantly enhanced the performance of organic yellow pigment PY181, making this method a practical modification approach. This method provides a novel way of improving the electrophoretic performance of color pigment particles that are challenging to directly connect with an ionic liquid, leading to the improved electrophoretic mobility of pigment particles. It is suitable for the surface modification of various pigment particles.