The influence of wind stress, small-scale waves, and surface films on air-sea gas exchange at low to moderate wind speeds (<10 m s?1) is examined. Coincident observations of wind stress, heat transfer velocity, surface wave slope, and surface film enrichments were made in coastal and offshore waters south of Cape Cod, New England, in July 1997 as part of the NSF-CoOP Coastal Air-Sea Chemical Fluxes study. Gas transfer velocities have been extrapolated from aqueous heat transfer velocities derived from infrared imagery and direct covariance and bulk heat flux estimates. Gas transfer velocity is found to follow a quadratic relationship with wind speed, which accounts for ~75–77% of the variance but which overpredicts transfer velocity in the presence of surface films. The dependence on wind stress as represented by the friction velocity is also nonlinear, reflecting a wave field-dependent transition between limiting transport regimes. In contrast, the dependence on mean square slope computed for the wave number range of 40–800 rad m?1 is found to be linear and in agreement with results from previous laboratory wind wave studies. The slope spectrum of the small-scale waves and the gas transfer velocity are attenuated in the presence of surface films. Observations over large-scale gradients of biological productivity and dissolved organic matter show that the reduction in slope and transfer velocity are more clearly correlated with surface film enrichments than with bulk organic matter concentrations. The mean square slope parameterization explains ~89–95% of the observed variance in the data and does not overpredict transfer velocities where films are present. While the specific relationships between gas transfer velocity and wind speed or mean square slope vary slightly with the choice of Schmidt number exponent used to scale the heat transfer velocities to gas transfer velocities, the correlation of heat or gas transfer velocity with mean square slope is consistently better than with wind speed.