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Abstract Dispersion processes in the ocean surface boundary layer (OSBL) determine marine material distributions such as those of plankton and pollutants. Sheared velocities drive shear dispersion, which is traditionally assumed to be due to mean horizontal currents that decrease from the surface. However, OSBL turbulence supports along-wind jets; located in near-surface convergence and downwelling regions, such turbulent jets contain strong local shear. Through wind-driven idealized and large-eddy simulation (LES) models of the OSBL, this study examines the role of turbulent along-wind jets in dispersing material. In the idealized model, turbulent jets are generated by prescribed cellular flow with surface convergence and associated downwelling regions. Numeric and analytic model solutions reveal that horizontal jets substantially contribute to along-wind dispersion for sufficiently strong cellular flows and exceed contributions due to vertical mean shear for buoyant surface-trapped material. However, surface convergence regions also accumulate surface-trapped material, reducing shear dispersion by jets. Turbulence resolving LES results of a coastal depth-limited ocean agree qualitatively with the idealized model and reveal long-lived coherent jet structures that are necessary for effective jet dispersion. These coastal results indicate substantial jet contributions to along-wind dispersion. However, jet dispersion is likely less effective in the open ocean because jets are shorter lived, less organized, and distorted due to spiraling Ekman currents.