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Abstract The fate and aggregation of nanoparticles (NPs) in the subsurface are important due to potentially harmful impacts on the environment and human health. This study aims to investigate the effects of flow velocity, particle size, and particle concentration on the aggregation rate of NPs in a diffusion-limited regime and build an equation to predict the aggregation rate when NPs move in the pore space between randomly packed spheres (including mono-disperse, bi-disperse, and tri-disperse spheres). The flow of 0.2 M potassium chloride (KCl) through the random sphere packings was simulated by the lattice Boltzmann method (LBM). The movement and aggregation of cerium oxide (CeO₂) particles were then examined by using a Lagrangian particle tracking method based on a force balance approach. This method relied on Newton's second law of motion and took the interaction forces among particles into account. The aggregation rate of NPs was found to depend linearly on time, and the slope of the line was a power function of the particle concentration, the Reynolds (Re) and Schmidt (Sc) numbers. The exponent for theScnumber was triple that of theRenumber, which was evidence that the random movement of NPs has a much stronger effect on the rate of diffusion-controlled aggregation than the convection.