Electrorheological (ER) fluid, as an intelligent material, is a kind of suspension composed of polarized micro‐ and/or nanoparticles dispersed into insulating oil. In recent years, molybdenum disulfide (MoS2), as the hottest 2D material, has provided a new strategy to develop the high‐performance ER materials. 2D‐based ER composites can provide large surface to enhance the polarization. But the MoS2 ER material has many disadvantages such as low polarization strength and high electrical conductivity. To make up these defects, polyaniline (PANI) is used to combine with lamellar MoS2. Herein, PANI and MoS2 hybrid composite nanoparticles with special morphology are prepared by two‐step method. The coating material has special morphology, high interfacial polarization, specific surface area, and low density. The optimum reaction ratio is obtained by adjusting the proportion of MoS2 and PANI. When the proportion of PANI and MoS2 is 4:1, the material performance is best, in which the shear stresses can reach 150 Pa. In a word, it is proved that the material is an excellent electrorheological material.
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