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Abstract Magnetorheological fluids (MRF) are smart materials of increasing interest due to their great versatility in mechanical and mechatronic systems. As main rheological features, MRFs must present low viscosity in the absence of magnetic field (0.1–1.0 Pa.s) and high yield stress (50–100 kPa) when magnetized, in order to optimize the magnetorheological effect. Such properties, in turn, are directly influenced by the composition, volume fraction, size, and size distribution (polydispersity) of the particles, the latter being an important piece in the improvement of these main properties. In this context, the present work aims to analyze, through experiments and simulations, the influence of polydispersity on the maximum packing fraction, on the yield stress under field (on-state) and on the plastic viscosity in the absence of field (off-state) of concentrated MRF (φ= 48.5 vol.%). Three blends of carbonyl iron powder (CIP) in polyalphaolefin oil were prepared. These blends have the same mode, but different polydispersity indexes (α), ranging from 0.46 to 1.44. Separate simulations show that the random close packing fraction increases from about 68% to 80% as the polydispersity indexes increase over this range. The on-state yield stress, in turn, is raised from 30 ± 0.5 kPa to 42 ± 2 kPa (B≈ 0.57 T) and the off-state plastic viscosity, is reduced from 4.8 Pa.s to 0.5 Pa.s. Widening the size distributions, as is well known in the literature, increases packing efficiency and reduces the viscosity of concentrated dispersions, but beyond that, it proved to be a viable way to increase the magnetorheological effect of concentrated MRF. The Brouwers model, which considers the void fraction in suspensions of particles with lognormal distribution, was proposed as a possible hypothesis to explain the increase in yield stress under magnetic field.