The effects of both hydrodynamic interaction and the form of the interparticle potential on the aggregation process for dispersed spherical particles are investigated by computational simulation. The simulation methods of Brownian Dynamics (BD) and Stokesian Dynamics (SD) are applied, over a range of solid volume fraction of 0.04 <= phi <= 0.12. The interparticle potential is a combination of a generalized Lennard-Jones form and a Yukawa potential, the latter of which describes a screened electrostatic repulsion at longer range. The combined potential is parameterized to include a roughly constant primary minimum near contact, along with a variable repulsive barrier at slightly larger separation. The microstructure is characterized through the pair distribution function, g(r), and the static structure factor. The repulsive barrier reduces the rate of aggregation and is also seen to affect the structure, with a large repulsion associated with a more tenuous structure. This is reflected in the potential having a strong effect on the evolution of 'bonds' per particle. Hydrodynamic interactions were found to reduce the solid fraction required for percolation, with the influence depending upon the form of the potential; the difference in percolation threshold was significant, with phi(c,SD)(=) over dot0.06 and phi(c,BD) >= 0.08 a typical difference for moderate repulsion barriers. These results are for 864 particles in a cubic unit cell. To address the mechanism for this influence of hydrodynamic interactions, a complementary analysis of the evolution of numerous independent three-particle aggregates was performed. The analysis shows that hydrodynamic interaction slows the evolution toward a condensed aggregate of lowest potential energy in a way which cannot be explained by a simple rescaling of the drag due to uncorrelated particle motions. (C) 2011 Elsevier Inc. All rights reserved.