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Surface modified carbonyl iron particles (SMCIPs) were synthesized by coating carbonyl iron particles with an organic reagent (N-polyether, N, N, N,-acetyloxy) 2, 6-aminion-1, 3, 4-thiadiazole dimer. The properties of these SMCIPs, including morphology, structure, and magnetic behavior, were characterized using scanning electron microscopy and a vibrating sample magnetometer. Aqueous magnetorheological (MR) fluids were prepared using SMCIPs. MR properties were measured via a strain-controlled parallel disk rheometer equipped with a magnetic field source. Addition of the organic surface coating layer was found to greatly improve sedimentation stability of the aqueous MR fluids at a small cost of a reduction in field dependent yield stress.