A magnetorheological fluid for use in magnetorheological ultrasmooth polishing of a substrate surface, comprising an aqueous carrier vehicle; a first amount of magnetic particles having a average diameter between about 1 micrometer and about 2 micrometers; and a second amount of abrasive particles having an average diameter between about <1 nanometer and about 15 nanometers. The fluid may further comprise a chemical stabilizer. Preferably the size of the magnetic particles is 2 to 3 orders of magnitude greater than the size of the abrasive particles. Preferably, the magnetic particles are spherical and include carbonyl iron, and preferably, the abrasive particles are selected from the group consisting of aluminum oxide, zirconium oxide, cerium oxide, silica, boron carbide, silicon carbide, natural diamond, synthetic diamond, and combinations thereof.
