Wind-erodible soil sediments are classified as aggregates and particles < 1 mm in diameter. Aggregate size has been reported to influence pesticide retention and behavior in the soil. Atrazine sorption and desorption isotherms were determined using batch equilibration methods for six aggregate sizes of Barnes loam (fine-loamy, mixed, superactive, frigid Calcic Haplodol) and Brandt silty clay loam (fine-silty, mixed, superactive, frigid Calcic Haplodol) soils. Aggregate and particle sizes used in this study ranged from < 0.11 to > 1.7 mm, and atrazine concentrations ranged from 0.65 to 39.2 μmol L−1. The Kf values for the isotherms were calculated using the Freundlich equation. In the Barnes loam, Kf values were strongly positively correlated to aggregate size, particle size, and organic carbon (OC) content (P = 0.01 for each parameter), whereas in the Brandt silty clay loam, Kf values were less correlated to size and OC content (P ≥ 0.1) but were better correlated to clay content and estimated specific surface area (P = 0.05 for each parameter). Desorption was hysteretic with about 18% more atrazine desorbed from smallest than from largest size fractions. At a concentration of 13.0 μmol L−1, the amount desorbed ranged from 9 to 13.7% of the initial amount of adsorbed atrazine after 5 d, whereas at 39.2 μmol L−1, the amount desorbed ranged from 10.3 to 16% of the amount adsorbed. These data indicate that wind-erodible size aggregates and particles could be a source of herbicide contamination of surface water.