Quantitative linkage of fundamental physicochemical characteristics to rate coefficients used in simulations of experimentally observed transport behaviors of nanoparticles and microplastics (colloids) in environmental granular media is an active area of research. Quantitative linkage is herein demonstrated for (i) colloids ranging from nano- to microscale; in two field-based granular media of contrasting grain size, (ii) natural fine sand at the column scale; and (ii) streambed-equilibrated commercial pea gravel at the field scale. Continuum-scale rate coefficients were linked to nanoscale interactions via mechanistic pore-scale colloid trajectory simulations that predicted and defined fast- and slow-attaching subpopulations, as well as nonattaching subpopulations that either remained in the near-surface pore water or re-entrained to bulk pore water. These subfractions of the classic collector efficiency were upscaled to continuum-scale rate coefficients that produced experimentally observed colloid breakthrough-elution concentration histories and nonexponential colloid distributions from the source. The simulations explained transition from hyperexponential to nonmonotonic colloid distributions from the source as driven accumulation of mobile near-surface colloids due to relatively strong secondary minimum interaction and weak diffusion for microscale colloids. The assumption of depletion of the fast-attaching colloid subpopulation by attachment to grain surfaces produced the experimentally observed contrasting distances across which nonexponential colloid distribution from the source occurred in the fine sand versus pea gravel. Rate coefficients were quantitatively calculated from physicochemical parameters and the following three fit parameters: (i) fractional coverage by nanoscale heterogeneity; (ii) efficiency of return to the near-surface domain; and (iii) in explicit simulations, characteristic velocity for scaling transfer to near-surface pore water.