A polymerization process to synthesize bimodal latexes with maximum particle diameters below 350 nm and solids content above 65 wt% has been developed. The process is based on an iterative strategy to determine the optimal particle size distribution that gives the maximum packing factor for a given range of particle sizes and at a given solids content. The calculated optimal bimodal PSD was experimentally obtained in a seeded semi-continuous emulsion polymerization reaction as follows: in the first step, a polymer seed latex was loaded in the reactor and grown, under monomer starved conditions, until a given particle size. At this point a fraction of the same seed was added to the reactor and the feed was continued until the desired particle size distribution and solids content were achieved. The point at which the seed was added again to the reactor and the amount of seed required were determined by the iterative strategy and depended on the competitive growth rate ratio of large and small particles that is an input for the iterative strategy. Implementation of the solution obtained from the iterative strategy, and for the first time in the open literature, led to the production of a coagulum free and stable bimodal latex with 70 wt% of solids content and particle sizes below 350 nm. (C) 2010 Elsevier Ltd. All rights reserved.