Fatty acid and organic carbon contents have been measured in the particulate and dissolved phases of surface microlayer and subsurface water samples collected from Lake Michigan. Concentrations are highest close to fluvial sources and lowest in offshore areas, yet surface/subsurface fractionation is lowest near river mouths and highest in open lake locations. These gradients plus accompanying fatty acid compositional changes indicate that river-borne organic materials are important constituents of coastal Lake Michigan microlayers and that sinking and turbulent resuspension of particulates affect surface film characteristics. Lake neuston and plankton contributes organic components which partially replace potamic materials removed by sinking.